Jones graduated from North Carolina Central University after a spectacular career there. He scored 1,770 points playing for Hall of Fame coach John McLendon. He was a 4-year letter winner and was a 3-time All-Conference team.
Jones was named to the All-NBA Second Team three straight years (1965–67) and he played on ten championship teams (1959-66 and 1968-69) — a total exceeded only by teammate Bill Russell in NBA history. He was 6-foot-4 (1.93 m) and weighed 200 lb (97 kg).
Jones was originally claimed by the Minneapolis Lakers, but returned to college upon completion of military service, and therefore voided NBA rules.
Jones’ perfect form when shooting a jump shot, along with his great clutch shooting led opponents to nickname him "The Shooter". At 6-foot-4, Jones was the prototype of the tall guard who could run the floor, bang the boards and had a rangy offensive game that gave opponents fits. One of the "Jones Boys" in Boston, Sam teamed with K.C. Jones in the Celtics' backcourt to create havoc in NBA arenas around the country.
He led Boston in scoring in the 1962-63 NBA season (19.7 points per game), 1964-65 NBA season (25.9) and 1965-66 NBA season (23.5). He produced four consecutive seasons averaging 20 points or better (1965–68). He owns Boston's fourth best single-game scoring output (51 points vs. Detroit Pistons on October 29, 1965). He scored 2,909 points in 154 playoff games (18.9 ppg), 15th best in history.