She was known for her innovations in fashion photography, World War II photographs, and portraits of famous Americans, Europeans, children, and women from all walks of life.

Familiar with many of the families and sports of the upper class, she began to photograph sportsmen and women in such fields as golf and sailing.

Toni and her husband purchased a large, white house on Long Island at Saint James called 'Sherrewogue'.

She was fired because of her poor spelling, but was encouraged by Vogue’s fashion editor Carmel Snow to take up photography.

She used it to cope with the illness of her mother, the death of her brother Varick Frissell, and the end of her engagement to Count Serge Orloff-Davidoff.

On behalf of the War Department and the Red Cross, she took thousands of images of nurses, front-line soldiers, WACs, African-American airmen, and orphaned children.

[citation needed] During the War she produced a series of photographs of children that were used in an edition of Robert Louis Stevenson's much-published A child's garden of verses.

In the 1950s, Frissell took informal portraits of the famous and powerful in the United States and Europe, including Winston Churchill, Eleanor Roosevelt, the Vanderbilts,[9] architect Stanford White[5] and John F. and Jacqueline Kennedy.

When she grew tired of fashion photography and fluctuating between contracts with Vogue and Harper’s Bazaar, she continued her interest in active women and sports.

[14] In 1966 Life magazine paid tribute to her in a page 3 editorial profile, headed "Patrician Photographer of a Vanishing Age".

Like Martin Munkacsi, she mastered the appearance of unselfconscious spontaneity in fashion pictures by working outside and on location with her models.

She had a tendency to use uncommon perspectives, which she achieved by placing her camera on a dramatic diagonal axis, and/or using a low point of view and a wide-angle lens against a neutral background, thus creating the illusion of elongated human form.

With her preference for close-ups and straightforward, unembellished images of winsome, sportswear-clad models, Frissell's action-fashion photographs are landmarks in the development of postwar fashion imagery.