episode "The He-She Chemistry" of Craig Stevens's CBS drama Mr. Broadway. She made two appearances on the early '60s TV series Route 66. On May 16, 1960, Grimes acted and sang as Mehitabel in an abridged version of the musical Archy and Mehitabel as part of the syndicated TV anthology series Play of the Week presented by David Susskind, and co-written by Mel Brooks and Joe Darion. The cast included Eddie Bracken (who reprised the role in the 1970 animated feature version Shinbone Alley with Carol Channing in the Mehitabel role) and Jules Munshin. Grimes was originally chosen to play the part given to Elizabeth Montgomery in the hit television situation comedy Bewitched, but she turned down the offer, preferring to star in The Tammy Grimes Show. She appeared in the television drama Route 66 on December 13, 1963, in an episode titled "Come Home Greta Inger Gruenschaffen". In 1964, she appeared on Broadway as Elvira Condomine in High Spirits, a musical version of Noel Coward's Blithe Spirit. In 1966, Grimes starred in her own ABC television series, The Tammy Grimes Show, in which she played a modern-day heiress who loved to spend money. Receiving unfavorable critical reaction and poor ratings, it ran for only a month, although an additional six episodes had already been made. Returning to the Broadway stage in 1969 after almost a decade of performing in what The New York Times called "dubious delights", Grimes appeared in a revival of Noël Coward's Private Lives as Amanda, winning the Tony Award for Best Actress. Clive Barnes in a New York Times review called her performance "outrageously appealing. She plays every cheap trick in the histrionic book with supreme aplomb and adorable confidence. Her voice moans, purrs, splutters; she gesticulates with her eyes, almost shouts with her hair. She is all campy, impossible woman, a lovable phony with the hint of tigress about her, so ridiculously artificial that she just has to be for real." She was a member of the Stratford Festival of Canada acting company in 1956, and returned again in 1982 to appear as Madame Arcati in Blithe Spirit. In addition to appearing in a number of television series and motion pictures, Grimes also entertained at various New York City night clubs and recorded several albums of songs. She recited poetry as part of a 1968 solo act in the Persian Room of the Plaza