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Molybdenum disulfide (MoS2) has been recognized as one of the most promising candidates to replace precious Pt for hydrogen evolution reaction (HER) catalysis, due to the natural abundance, low cost, tunable electronic properties, and excellent chemical stability. Although notable processes have been achieved in the past decades, their performance is still far less than that of Pt. Searching effective strategies to boosting their HER performance is still the primary goal. In this review, the recent process of the electronic regulation of MoS2 for HER is summarized, including band structure engineering, electronic state modulation, orbital orientation regulation, interface engineering. Last, the key challenges and opportunities in the development of MoS2-based materials for electrochemical HER are also discussed.