She appeared in the original Broadway production of The Most Happy Fella and later played the role of Elizaveta in Grand Hotel. Her many other stage credits include Sweet Charity, Oklahoma!, Damn Yankees!, Carnival, and The Owl and the Pussycat.
In addition, she worked frequently in television and movies, with credits including Guiding Light, Sunrise at Campobello, The Doctors and the Nurses, Emergency!, and Santa Barbara.
Bethune was a dancer at New York City Ballet in her teens, and later danced with The Royal Danish Ballet, The San Francisco Ballet, and her own company, Zina Bethune and Company.