MoS2/carbon hybrid materials have been shown to be promising non-precious metal electrocatalysts for the hydrogen evolution reaction (HER). However, a facile method for synthesizing them is still a big challenge, let alone patterning them through a design. In this work, we present a novel strategy to synthesize and pattern MoS2/carbon hybrid materials as electrocatalysts for the HER through a one-step direct laser writing (DLW) method under ambient conditions. DLW on citric acid–Mo–S precursors leads to the in situ synthesis of small-sized MoS2 nanoparticles (NPs) anchored to the carbon matrix. Largely exposed catalytically active sites from the MoS2 NPs and the synergetic effect from the carbon matrix make the hybrid materials exhibit superior catalytic performance and stability for the HER in acidic solutions. Through computer-controlled laser beams we can design arbitrary patterns made of these catalysts on targeted substrates, which will open a new route for fabricating on-chip microfuel cells or catalytic microreactors.