We directly synthesize MoWS nanosheets on conductive carbon nanotube yarn (MoWS/CNTY) and carbon fiber cloth (MoWS/CC) through a fast and low-temperature thermolysis method in order 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 are achieved for MoWS/CC and MoWS/CNTY, respectively, by optimizing the density of the exposed active edge sites of vertically aligned MoWS 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.