We directly synthesize MoWS₂ nanosheets on conductive carbon nanotube yarn (MoWS₂/CNTY) and carbon fiber cloth (MoWS₂/CC) through a fast and low-temperature thermolysis method to obtain flexible catalyst electrodes that show high performance in the hydrogen evolution reaction. Small Tafel slopes of 41.8 and 46.7 mV dec^–1 are achieved for MoWS₂/CC and MoWS₂/CNTY, respectively, by optimizing the density of the exposed active edge sites of vertically aligned MoWS₂ on CNTY and CC. Furthermore, the catalyst electrodes demonstrate good electrocatalytic stability over 36 h. The proposed technique for fabricating high-performance, binder-free, and flexible catalyst electrodes is more accessible and faster than conventional methods.