Yeats introduced Smith to the Hermetic Order of the Golden Dawn, which she joined in 1901 and in the process met Waite. When the Golden Dawn splintered due to personality conflicts, Smith moved with Waite to the Independent and Rectified Rite of the Golden Dawn (or Holy Order of the Golden Dawn). In 1909, Waite commissioned Smith to produce a tarot deck with appeal to the world of art, and the result was the unique Waite-Smith tarot deck. Published by William Rider & Son of London, it has endured as the world’s most popular 78-card tarot deck. The innovative cards depict full scenes with figures and symbols on all of the cards including the pips, and Smith’s distinctive drawings have become the basis for the design of many subsequent packs
In 1907, Alfred Stieglitz gave Smith an exhibition of paintings in New York at his Little Galleries of the Photo-Secession (also known as gallery 291), making Smith the first painter to have a show at what had been until then a gallery devoted exclusively to the photographic avant-garde. Stieglitz was intrigued by Smith’s synaesthetic sensibility; in this period, Smith would paint visions that came to her while listening to music.