In November 1915 Connolly appointed her secretary of the Irish Women Workers' Union, in succession to Delia Larkin. This union had been formed during the strike at Jacob's Biscuit Factory 1911 and was part of the 1913 Dublin Lock-out. 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, Molony describes leafletting O'Connell Street – then, on the GPO side, only frequented by British soldiers and their mots: "Misses Elizabeth O'Farrell and Sighle Grennan and myself were spotted by police. We took to our heels, and were chased through Henry Street, Mary Street and right up to the Markets in Capel Street. We got away clear, as we were young and swift, and the police were hampered by long heavy overcoats. On the whole we feared more the soldiers with their canes." Fianna Éireann, the cadet body of the Irish Volunteers, was founded by Constance Markievicz in Molony's home at 34 Lower Camden Street, Dublin, on 16 August 1909. . 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 confined to a friend in the 1930s that she believed they were to be wed, but that Hobson had 'broken her heart' and left her. Molony was a prominent member of Cumann na mBan, a republican women's paramilitary organisation formed in April 1914 as an auxiliary of the Irish Volunteers.