In this study, we report nonmetal plasmonic MoS2@TiO2 heterostructures for highly efficient photocatalytic H2 generation. Large area laminated MoS2 in conjunction with TiO2 nanocavity arrays is achieved via carefully controlled anodization, physical vapor deposition, and chemical vapor deposition processes. The broad spectral response ranging from ultraviolet-visible (UV-vis) to near-infrared (NIR) wavelengths and finite element frequency-domain simulations suggest that this MoS2@TiO2 heterostructure enhances photocatalytic activity for H+ reduction. A high H2 yield rate of 181 μmol h−1 cm−2 (equal to 580 mmol h−1 g−1 based on the loading mass of MoS2) is achieved using a low catalyst loading mass. The spatially uniform heterostructure, correlated with plasmon-resonance through the conformal MoS2 coating that effectively regulates charge transfer pathways, is proven to be vitally important for the unique solar energy harvesting and photocatalytic H2 production. As an innovative exploration, our study demonstrates that the photocatalytic activities of nonmetal, earth-abundant materials can be enhanced with plasmonic effects, which may serve as an excellent catalytic agent for solar energy conversion to chemical fuels.