The search for efficient, earth-abundant electrocatalysts for the hydrogen evolution reaction (HER) has identified unsaturated molybdenum disulfide (MoS2) as a leading candidate. This review synthesises recent advancements in the engineering of MoS2 to enhance its electrocatalytic properties. It focuses on strategies for designing an unsaturated electronic structure on metal catalytic centers and their role in boosting the efficiency of the hydrogen evolution reaction (HER). It also considers how to optimize the electronic structures of unsaturated MoS2 for enhanced catalytic performance. This review commences with an examination of the fundamental crystal structure of MoS2; it elucidates the classical unsaturated electron configurations and the intrinsic factors that contribute to such electronic structures. Furthermore, it introduces popular strategies for constructing unsaturated electronic structures at the atomic level, such as nanostructure engineering, surface chemical modification and interlayer coupling engineering. It also discusses the challenges and future research directions in the study of MoS2 electronic structures, with the aim of broadening their application in sustainable hydrogen production.
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