The former lieutenant governor, whose health had been in decline, died in Los Angeles, his wife Alice Gueno Dymally said in a statement.
"He lived a very extraordinary life and had no regrets," Mrs. Dymally said.
The Trinidad-born Dymally was a former janitor, union organizer and teacher before entering politics in 1963, where he served in both houses of the state Legislature and in Congress representing Compton and its surrounding area.
He was elected as the state's first foreign-born black assemblyman in 1962, the first black senator in 1966, the first and only black lieutenant governor in 1974 and went on to win his congressional seat in 1980. In Congress, he served as chairman of the Congressional Black Caucus and the House Foreign Affairs Committee where he championed economic and humanitarian aid for Africa.
He took a 10-year retirement before running again at age 76 for the Assembly seat he held at the start of his political career. He won two more terms and ran, at 82, for the state Senate again in 2008, but lost the Democratic primary to Rod Wright.
During his time in politics Dymally was also tainted by numerous investigations of fraud, bribery and pay-for-play campaign contributions.
Such allegations, including unsubstantiated claims he would be indicted by the federal government, eventually led to his defeat in his 1978 bid for re-election as lieutenant governor.
Dymally maintained that he never acted illegally and said the probes were politically motivated. No charges were ever filed.
"We politicians ... think we are very important, but we are not that important, and regular people don't seem to be that concerned about a lot of the legislation that we pass," he told the Associated Press in a 2002 interview. "My legacy has not been my legislation. My legacy has been my openness."
In his final years, the tireless Dymally lead a health institute at the Charles Drew University of Medicine and Science in South Los Angeles. The university's nursing school bears his name.
"His dedication to public service continued when he left politics and his legacy will be long remembered," Lt. Gov. Gavin Newsom said in a statement. He called Dymally "a trailblazer in every sense of the word."
Besides his wife, Dymally was survived by his son Mark and daughter Lynn.
Plans for a memorial service were pending.