Molony also had a career as an actress, and was a member of the
Abbey Theatre. However her primary commitment was to her political work. She was a strong political influence, credited with bringing many into the movement, including Constance Markievicz and Dr
Kathleen Lynn, who wrote: ‘We used to have long talks and she converted me to the national movement. She was a very clever and attractive girl with a tremendous power of making friends.’ In November 1915 Connolly appointed her secretary of the
Irish Women Workers' Union, in succession to
Delia Larkin. Molony managed the union's shirt factory in Liberty Hall, founded to give employment to the strikers put out of work and blacklisted after the strike. "Not one of them is a penny the better for her part in either fight [the 1916 Rising, where all served, and the strike at Jacob's]," wrote Molony in her statement to the Bureau of Military History. "In such a manner is the real aristocracy of a country born." She was friendly with the family of
Thomas MacDonagh and his wife, Muriel, and was the godmother of their daughter Barbara, whose godfather was
Patrick Pearse; describing Liberty Hall, where Connolly spent much of his time, she wrote: "Connolly, after hours, could be free for private visitors… Pearse called many times, also Joe Plunkett and Tom MacDonagh. These men were all intimate friends of mine, so it seemed quite natural for me to encourage them to buy socks and ties from us." In the same account, Markievicz worked closely with Molony and
Bulmer Hobson in organising the fledgling Fianna. It was during this period of working together in building the Fianna that Molony and Hobson grew close and became romantically linked. However, the relationship was not to last. Molony confided to a friend in the 1930s that she believed they were to be wed, but that Hobson had 'broken her heart' and left her. ==1916 Easter Rising==