Amorphous MoSx thin-film-coated carbon fiber paper as a binder-free 3D electrode was synthesized by a facile hydrothermal method. The maximum specific capacitance of a single electrode was 83.9 mF cm-2, while it was 41.9 mF cm-2 for the symmetric device. Up to 600% capacitance retention was observed for 4750 cycles.