A litchi-like MoSx-Fe@UiO-66-(OH)2 nanocomposite with amorphous MoSx-Fe nanoparticles uniformly anchored on the surface of UiO-66-(OH)2 is synthesized through sequential room-temperature redox and coordination reaction. The composite exhibits high catalytic activity and durability for hydrogen evolution in an acidic electrolyte, delivering 1000 mA cm-2 at -297 mV and outperforming Pt/C under high current densities.