David Ehrenstein, author of the book Open Secret: Gay Hollywood, 1928–2000, said that Smith was openly gay and, as a result, did not pursue a Hollywood career.

Tucker Smith was an American Theatre Wing scholarship winner and he first moved to New York City from his native Philadelphia in September 1955. Shortly afterward, he joined the national tour of Damn Yankees. In 1958 he joined the cast of the original Broadway production of West Side Story, as a replacement for the role of Big Deal, then going on to play the roles of Diesel and Snowboy. He understudied for the character of Riff and had played that role many times. The musical went on a national tour in the United States from June 14, 1959‚ to April 23, 1960‚ and Smith went along with it.

After the film, Smith continued his association with West Side Story. He played Riff in both the 1962 Los Angeles and 1963 Sacramento productions of the musical, the latter with Sylvia Lewis in the role of Anita. He reprised the role again in 1964, when West Side Story went on tour in Tokyo, Japan. Right before West Side Story's tour in Japan, Smith had performed at the 1964 New York World's Fair at the DuPont Pavilion in the musical The Wonderful World of Chemistry. That same year, Smith was in the cast for the Broadway musical Anyone Can Whistle. After a pre-Broadway run in Philadelphia, the show closed after a week and only nine performances.

In the 1970s Smith owned and operated a bar named “Tucker’s Turf” in North Hollywood.

Smith went on to perform at other venues, including Las Vegas shows, nightclubs, cabarets, and stage productions both in the United States and abroad. His stage work includes Parade with Carole Cook and Michele Lee, Vintage '60, also with Michele Lee and Sylvia Lewis, the San Francisco production of Half a Sixpence" with Anne Rogers and Roger C. Carmel, and the 1973 musical version of Gone With the Wind, which was choreographed by Joe Layton. Smith had toured with Carol Channing in her 1970 revue "Carol Channing with Her 10 Stout-Hearted Men‚" which was also choreographed by Joe Layton. Finally, Smith had also toured internationally with his own nightclub act.

Tucker Smith died of cancer on December 22, 1988‚ at the age of 52 at the UCLA Medical Center in Los Angeles, California. His cancer has been attributed by various sources as to be throat, neck and/or jaw cancer, and was diagnosed in late 1986. At the time of his death, Smith was survived by three sisters. Some newspapers erroneously printed that he was survived by three daughters. After his death, Smith was laid to rest in his hometown of Philadelphia.

Smith was one of the several cast members from the Broadway production that were chosen to appear in the movie version of West Side Story. He was contracted to play Ice, a role newly created for the movie. In the film, Smith was the singer and central performer of the pivotal song “Cool‚” originally sung by the character of Riff in the Broadway musical. Besides performing “Cool‚” Smith would also dub some of Russ Tamblyn’s singing in “Jet Song.”