Returning to the United Kingdom, she made her film debut with a starring role in an early Alfred Hitchcock film The Skin Game (1931), and over the next few years appeared in several British and (pre-Code) Hollywood films, including Thirteen Women (1932).
Thayer also wrote several novels, including the bestseller Thirteen Women (1930) which was filmed as Thirteen Women (1932) and released by RKO Radio Pictures.
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In 1978, she organized a team of thirteen women to climb Annapurna (I) in Nepal which, until then, had been climbed by only eight people (all men).