Defect engineering is one of the effective strategies to optimize the physical and chemical properties of molybdenum disulfide (MoS 2 ) to improve catalytic hydrogen evolution reaction (HER) performance. Dislocations, as a typical defect structure, are worthy of further investigation due to the versatility and sophistication of structures and the influence of local strain effects on the catalytic performance. Herein, this study adopted a low-temperature hydrothermal synthesis strategy to introduce numerous dislocation-strained structures into the in-plane and out-of-plane of MoS 2 nanosheets. Superior HER catalytic activity of 5.85 mmol·g −1 ·h −1 under visible light was achieved based on the high-density dislocations and the corresponding strain field. This work paves a new pathway for improving the catalytic activity of MoS 2 via a dislocation-strained synergistic modulation strategy.