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Engineering electronic properties is a promising way to design nonprecious-metal or earth-abundant catalysts toward hydrogen evolution reaction (HER). Herein, we deposited catalytically active MoS₂ flakes onto black phosphorus (BP) nanosheets to construct the MoS₂–BP interfaces. In this case, electrons flew from BP to MoS₂ in MoS₂–BP nanosheets because of the higher Fermi level of BP than that of MoS₂. MoS₂–BP nanosheets exhibited remarkable HER performance with an overpotential of 85 mV at 10 mA cm^–2. Due to the electron donation from BP to MoS₂, the exchange current density of MoS₂–BP reached 0.66 mA cm^–2, which was 22 times higher than that of MoS₂. In addition, both the consecutive cyclic voltammetry and potentiostatic tests revealed the outstanding electrocatalytic stability of MoS₂–BP nanosheets. Our finding not only provides a superior HER catalyst, but also presents a …