Bond was first elected to the Georgia House of Representatives in 1965 for a one-year term, but members of the House voted not to seat him due to his outspoken opposition to the Vietnam War. He won a second election one year later and again the Georgia House barred him from membership. After Bond won a third election, for a two-year term, the United States Supreme Court ruled that the Georgia House had violated Bond's rights in refusing him his seat.
He was elected to the State Senate in 1974 and left office in 1987, having served four terms in the House and six terms in the Senate. In the Senate, Bond became the first black chair of the Fulton County Senate Delegation, chairman of the Committee on Consumer Affairs, and a member of the committees on Human Resources, Governmental Operations, and Children and Youth.
In 1968, Bond was co-chairman of the Georgia Loyal National delegation to the Democratic convention. He was nominated for vice-president of the United States, the first black to be honored by a major political party. He withdrew his name because he was too young to serve.
Bond has served four terms on the NAACP national board, and in 1998 was elected its chairman. He was president of the Atlanta NAACP from 1978-1989.
Bond has been host and commentator on "America's Black Forum," the oldest black-owned show in television syndication, since 1980. He has been a commentator on the "Today" show and was the author of a nationally syndicated newspaper column called Viewpoint.
Time Magazine named Bond on its 200 Leaders List. He received the 1985 Bill of Rights Award from the American Civil Liberties Union of Georgia and a similar award from the Massachusetts Civil Liberties Union in 1990. In 1984, he received the Legislative Service Award from the Georgia Municipal Association.
A collection of Bond's essays has been published under the title A Time To Speak, A Time To Act. His poems and articles have appeared in such places as The Nation, Negro Digest, Motive, Life, Playboy, Exposure, The New York Times, New Negro Poets, The Book of Negro Humor, and The Los Angeles Times.
Bond has been a Pappas Fellow at the University of Pennsylvania and has served as visiting professor at Drexel University, Harvard University, and Williams College. He is currently a Distinguished Scholar in Residence at the American University in Washington, D.C., and a faculty member at the University of Virginia in the department of history.