As a teenager, Ayrton became deeply involved in the women's suffrage movement, joining the WSPU in 1907 after attending a celebration with released prisoners. In 1909 Ayrton opened the second day of the Knightsbridge "Women's Exhibition and Sale of Work in the Colours" which included new model bicycles painted in purple, white and green and raised from 50 stalls and tea etc. £5,664 for the movement. Ayrton was with the delegation that went with Emily Pankhurst to see the Prime Minister and met his private secretary instead on 18 November 1910 (Black Friday). Ayrton permitted Christabel Pankhurst to transfer sums to her bank account to avoid confiscation in 1912, and hosted Pankhurst in times of recovery from imprisonment and force feeding. One attempt to re-arrest Pankhurst on 29 April 1913 to continue her sentence was driven back by suffragettes picketing outside, but Pankhurst was eventually re-arrested outside Ayrton's home on her way to the funeral of Emily Davison (who was killed after running in front of the King's horse at the Derby).