Large‐scale production of hydrogen from water‐alkali electrolyzers is impeded by the sluggish kinetics of hydrogen evolution reaction (HER) electrocatalysts. The hybridization of an acid‐active HER catalyst with a cocatalyst at the nanoscale helps boost HER kinetics in alkaline media. Here, it is demonstrated that 1T–MoS
2 nanosheet edges (instead of basal planes) decorated by metal hydroxides form highly active
/
heterostructures, which significantly enhance HER performance in alkaline media. Featured with rich
/
sites, the fabricated 1T–MoS
2 QS/Ni(OH)
2 hybrid (quantum sized 1T–MoS
2 sheets decorated with Ni(OH)
2 via interface engineering) only requires overpotentials of 57 and 112 mV to drive HER current densities of 10 and 100 mA cm
?2, respectively, and has a low Tafel slope of 30 mV dec
?1 in 1 m KOH. So far, this is the best performance for MoS
2‐based electrocatalysts and the 1T–MoS
2 QS/Ni(OH)
2 hybrid is among the best‐performing non‐Pt alkaline HER electrocatalysts known. The HER process is durable for 100 h at current densities up to 500 mA cm
?2. This work not only provides an active, cost‐effective, and robust alkaline HER electrocatalyst, but also demonstrates a design strategy for preparing high‐performance catalysts based on edge‐rich 2D quantum sheets for other catalytic reactions.
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