The Brit, who portrays Daphne Bridgerton in the Netflix hit, fronts the new Fall 2021 advertisements for London-based label Self-Portrait, although Dynevor admits she found the experience a little strange as an actress.
Confessing posing for the photos was "weird", she told Britain's The Times, "I had to stay very still, so I had to rein it back."
However, Dynevor is a big fan of the brand's style, and was company founder and creative director Han Chong's first choice to feature in the campaign.
"As I was designing this latest collection, I was thinking a lot about the British sensibility and that effortless approach to British style, which I am so often inspired by," he told WWD.com.
"I felt we needed to work with someone to bring this to life rather than present the collection in a traditional show format, and having captured the hearts and imaginations of so many people over the last few months, I knew Phoebe would be the perfect woman."
Recalling how she first discovered Self-Portrait on the set of a photoshoot, Dynevor said, "[It was] an instant love affair. I love the strong structures he creates from such delicate and stunning fabrics and this collection is a testament to his incredible work. I'm so proud to be a part of this new project and hope to have a chance to wear the pieces when life goes back to normal again."