The exploration and scalable synthesis of the earth-abundant and excellent electrocatalysts without noble metal are crucial to the future hydrogen production and application. Herein, an affordable electrocatalyst is built through an in-situ growth of MoS 2 nanosheets vertically on the electro-exfoliated black phosphorus (EEBP) for hydrogen evolution reaction (HER). The electro-exfoliation achieves the high-yield production of fewlayer BP lamellae from its bulk crystal, hosting the scalable synthesis of uniform MoS 2 /EEBP heterostructure. Moreover, the vertical growth manner can effectively aggrandize the exposed MoS 2 edge sites and probably advance the catalytic activity to a certain extent. As for HER, such a MoS 2 /EEBP heterostructure exhibits promising catalytic performance with low overpotentials of 126 mV, 237 mV and 258 mV at 10 mA cm À 2 (η 10 ) as well as low Tafel slopes in both acid, alkaline and neutral media, respectively. The rationales behind the satisfactory catalytic properties are explained by density functional theory (DFT) calculations. Theoretically, it is revealed that the MoS 2 /EEBP heterostructure with a more neutral hydrogen adsorption energy can benefit the electrons migration and boost the water dissociation kinetics. This study presents an effective method to design and fabricate highly efficient heterostructure electrocatalysts through interface engineering towards hydrogen production.[a] T.