His role in 1968 movie Night of the Living Dead marked the first time an African-American actor was cast as the star of a horror film and one of the first times in American cinema where a person of color was given an important role when the script did not explicitly call for one. At the time, casting a black man as the hero of a film where all the other characters were white was potentially controversial. While some saw the casting as significant, the Director of the film states "Jones simply gave the best audition."

From 1972 to 1976, he oversaw the literature department at Antioch College. Jones was also a Phelps-Stokes exchange scholar in Niger and taught literature at Long Island University. He created English-language training programs for the Peace Corps and helped design Harlem Preparatory School, where he headed the English department.

He continued working in film after Night of the Living Dead. Jones was executive Director of the Black Theater Alliance, a federation of theater companies, from 1976 through 1981. He also taught acting styles at the American Academy of Dramatic Arts in New York City. As executive Director of the Richard Allen Center for Culture and Art (RACCA), he promoted African-American theater. After leaving the American Academy of Dramatic Arts he taught a select group of students privately in Manhattan, by invitation only. His hand-selected students were of diverse ethnic backgrounds. The students were picked from his Acting Styles classes at American Academy of Dramatic Arts.

Jones died of cardiopulmonary arrest at Winthrop-University Hospital in Mineola, Long Island, New York, on July 22, 1988, aged 51. He was cremated and his ashes given to his family.