Sterling died of natural causes following a decade-long battle with shingles, said his son, Jeffrey. His wife and other close relatives were at his bedside.
Although he appeared in dozens of movies, Sterling was best known for the 1953-1956 TV series "Topper," based on the Thorne Smith novel, and the 1937 film starring Cary Grant and Constance Bennett.
Sterling and Jeffreys played George and Marion Kerby, a fun-loving couple who were killed in an accident but returned as ghosts to haunt the new occupant of their home, a banker named Cosmo Topper.
Sterling was born William Hart in 1917 in New Castle, Pa., the son of Chicago Cubs catcher William S. Hart. He attended college in Pennsylvania and worked as a clothing salesman before breaking into movies.
He proved a versatile player, especially in romantic roles, and appeared in five films in 1941, including the romantic comedy "Two-Faced Woman" with Greta Garbo and "The Penalty" with Lionel Barrymore.
After "Topper," Sterling retired from acting to become a businessman.
Sterling was married to actress Ann Sothern from 1943 to 1949 and they had a daughter, actress Tisha Sterling. He married Jeffreys in 1951 and they had three sons: Jeffrey, Dana and Tyler.