In 1838, Henry Irby purchased 202 1/2 acres surrounding the present intersection of Peachtree, Roswell, and West Paces Ferry roads from Daniel Johnson for $650. Irby subsequently established a general store and tavern at the northwest corner of the intersection. The name "Buckhead" comes from a story that Irby killed a large buck deer and placed the head in a prominent location. Prior to this, the settlement was called Irbyville. By the late 1800s, Buckhead had become a rural vacation spot for wealthy Atlantans. In the 1890s, Buckhead was rechristened Atlanta Heights but by the 1920s it was again "Buckhead".

Buckhead remained dominated by country estates until after World War I, when many of Atlanta's wealthy began building mansions among the area's rolling hills. Simultaneously, a number of Black enclaves began popping up in Buckhead, following events like the 1906 Atlanta race riot and the Great Atlanta fire of 1917, which drove black residents from the city center. Predominantly black neighborhoods within Buckhead included Johnsontown, Piney Grove, Savagetown, and Macedonia Park.

Despite the stock market crash of 1929, lavish mansions were still constructed in Buckhead throughout the Great Depression. In 1930, Henry Aaron Alexander built one of the largest homes on Peachtree Road, a 15,000-square-foot (1,400 m) house with 33 rooms and 13 bathrooms. During the mid-1940s, Fulton County decided to acquire the land comprising Macedonia Park to build what is now Frankie Allen Park. This process, which entailed both eminent domain and "outright coercion" displaced over 400 families.

During the mid-1940s, Atlanta Mayor William B. Hartsfield sought to annex Buckhead, and a number of other predominantly White suburbs of Atlanta. Fearing that the city's "Negro population is growing by leaps and bounds", and was "taking more white territory inside Atlanta", Hartsfield sought to annex these communities to counteract the threat of increasing political power for the city's Black residents. The annexation of Buckhead was put to a vote in 1947, but it was rejected by Buckhead voters. Atlanta annexed Buckhead and a number of other nearby communities in 1952, following legislation which expanded Atlanta's city boundaries.

In 1956, an estate known as Joyeuse was chosen as the site for a major shopping center to be known as Lenox Square. The mall was designed by Joe Amisano, an architect who designed many of Atlanta's modernist buildings. When Lenox Square opened in 1959, it was one of the first malls in the country, and the largest shopping center in the Southeastern U.S. Office development soon followed with the construction of Tower Place in 1974.

To reverse a downturn in Buckhead Village during the 1980s, minimum parking spot requirements for bars were lifted, which quickly led to it becoming the most dense concentration of bars and clubs in the Atlanta area. Many bars and clubs catered mostly to the black community in the Atlanta area, including Otto's, Cobalt, 112, BAR, World Bar, Lulu's Bait Shack, Mako's, Tongue & Groove, Chaos, John Harvard's Brew House, Paradox, Frequency & Havana Club. The area became renowned as a party spot for Atlanta area rappers and singers, including Outkast, Jazze Pha, Jagged Edge, Usher and Jermaine Dupri, who mentioned the neighborhood's clubs on his song "Welcome to Atlanta".

Following the events of the Ray Lewis murder case in Buckhead on the night of the 2000 Super Bowl (held in Atlanta at the Georgia Dome), as well as a series of murders involving the Black Mafia Family, residents sought to ameliorate crime by taking measures to reduce the community's nightlife and re-establish a more residential character. The Buckhead Coalition's president and former Atlanta Mayor Sam Massell, along with councilwoman Mary Norwood were instrumental in persuading the Atlanta City Council to pass a local ordinance to close bars at 2:30 AM rather than 4 AM, and liquor licenses were made more difficult to obtain. Eventually, most of the Buckhead Village nightlife district was acquired for the "Buckhead Atlanta" multi-use project, and many of the former bars and clubs were razed in 2007.

In 2008, a newsletter by the Fulton County Taxpayers Foundation began circulating that proposed the secession of Buckhead into its own city after more than 50 years as part of Atlanta. This came on the heels of neighboring Sandy Springs, which finally became a city in late 2005 after a 30-year struggle to incorporate, and which triggered other such incorporations in metro Atlanta's northern suburbs. Like those cities, the argument to create a city of Buckhead is based on the desire for more local control and lower taxes.

Discussions revolving around potential secession from Atlanta were revived in late 2021, with proponents of secession arguing that splitting from Atlanta would enable Buckhead to better tackle crime in the area. In Atlanta's Police Zone 2, which includes Buckhead, Lenox Park, Piedmont Heights, and West Midtown, murder was up 63% in 2021 compared to the previous year, going from 8 cases to 13. However, in the same period crime overall was down by 6%, and according to police chief Rodney Bryant, Zone 2 had only a fraction of the violent crimes seen in other neighborhoods of Atlanta.

Buckhead, one of the wealthiest neighborhoods in Atlanta, would deprive the city of upwards of 40% of its tax revenue if it seceded. Political scientists and journalists have also highlighted that Buckhead is significantly more conservative and white than the rest of Atlanta. Commentators have also noted that this secession attempt is "more serious" than earlier efforts, due to polling data showing 54% to 70% of Buckhead's residents favor the move, and due to pro-secession organizations raising nearly $1,000,000 to promote the split. A referendum did not occur in 2022 or early 2023, as the Georgia General Assembly tabled the bills that would have provided for this referendum during the 2022 legislative session.

During the 2023 session, on April 27, the issue of incorporation was brought to the Georgia State Senate in the form of SB114. The bill prompted a response from governor Brian Kemp on the legality and workability of incorporating Buckhead as a city, but was ultimately rejected 33-23. The against votes consists of all Democrats in the Senate, and ten Republicans who broke rank to join them. Republicans on the for side argued that the citizens of Buckhead were not being represented by their municipal government and that the decision to form their own municipality should be up to the citizens themselves. Additionally, it was noted by the media that there was no Senator from Buckhead in the Senate at the time of the vote. If the bill succeeded, it would have begun the referendum process to secede from Atlanta.

Buckhead was originally the central area now called "Buckhead Village". The current usage of the term Buckhead roughly covers the interior of the "V" formed by Interstate 85 on the east and Interstate 75 on the west. Buckhead is bordered by Cumberland and Vinings in Cobb County to the northwest, the city of Sandy Springs to the north, Brookhaven and North Druid Hills in DeKalb County to the east, Midtown Atlanta to the south, and West Midtown to the west.

Buckhead comprises most of the neighborhoods of Atlanta's north side, 43 in total.

The southernmost area around the Brookwood and Ardmore neighborhoods is sometimes regarded as a separate neighborhood of "South Buckhead".

Since at least the 1950s, Buckhead has been known as a district of extreme wealth, with the western and northern neighborhoods being virtually unrivaled in the Southeast. In 2011, The Gadberry Group compiled the list of the 50 wealthiest zip codes in the United States, ranking Buckhead's western zip code (30327) as the second wealthiest zip code in the South (behind Palm Beach's 33480) and the second wealthiest zip code east of California and south of Virginia.

The same group reported the average household income at $280,631, with an average household net worth of $1,353,189. These 2011 figures are up from a similar 2005 study that pegged Buckhead as the wealthiest community in the South and the only settlement south of the Washington D.C. suburb of Great Falls, and east of the Phoenix suburb of Paradise Valley to be among the 50 wealthiest communities in the country. However, according to Forbes magazine, (30327) is the ninth-wealthiest zip code in the nation, with a household income in excess of $341,000.

The Robb Report magazine has consistently ranked Buckhead one of the nation's "10 Top Affluent Communities" due to "the most beautiful mansions, best shopping, and finest restaurants in the Southeastern United States". Due to its wealth, Buckhead is sometimes promoted as the "Beverly Hills of the East" or "Beverly Hills of the South" in reference to Beverly Hills, California, an area to which it is often compared.

Public schools in Buckhead are administered by Atlanta Public Schools.

The following public elementary schools serve Buckhead:

• Morris Brandon Elementary School
• Garden Hills Elementary School
• Warren T. Jackson Elementary School
• E. Rivers Elementary School
• Sarah Rawson Smith Elementary School

The area is served by Sutton Middle School and North Atlanta High School.

By 2012, due to overall population increases in Buckhead, many schools became increasingly crowded. Brandon Elementary was at 97% capacity, Garden Hills was at 102% capacity, E. Rivers was at 121% capacity, and Sutton was at 150% capacity. In the round of school zone change proposals in 2012, Ernie Suggs of The Atlanta Journal-Constitution said that the zones of Buckhead "remained pretty much intact."

There is an area charter school, Atlanta Classical Academy.

Local private schools include the Atlanta International School, the Atlanta Speech School, Christ the King School, the Atlanta Girls School, The Galloway School, Holy Spirit Preparatory School, Trinity School, The Lovett School, Pace Academy, and The Westminster Schools.

Georgia State University's J. Mack Robinson College of Business' Buckhead Center is located in the heart of Buckhead. This facility houses Georgia State's Executive MBA program. Its "Leadership Speaker Series", which showcases an agenda of executive officers from prestigious, well-known companies is also hosted at their Buckhead Center.

The University of Georgia's Terry College of Business Executive Education Center is located in Buckhead. This facility houses the university's executive MBA program and Terry Third Thursday, a lecture series featuring business leaders.

There are two branches of the Atlanta-Fulton Public Library System in Buckhead: Northside Branch and Buckhead Branch.