Sustainable hydrogen production via photocatalytic, electrocatalytic, and synergetic photoelectrocatalytic processes has been regarded as an effective strategy to address both energy and environmental crises. Due to their unique structures and properties, emerging ultrathin two-dimensional (2D) materials can bring about promising opportunities to realize high-efficiency hydrogen evolution. This review presents a critical appraisal of advantages and advancements for ultrathin 2D materials in catalytic hydrogen evolution, with an emphasis on structure–activity relationship. Furthermore, strategies for tailoring the microstructure, electronic structure, and local atomic arrangement, so as to further boost the hydrogen evolution activity, are discussed. Finally, we also present the existing challenges and future research directions regarding this promising field.

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DOI: 10.1016/j.mattod.2018.01.034