The activity and accessibility of MoS 2 edge sites are critical to deliver high hydrogen evolution reaction (HER) efficiency. Here, a porous carbon network confining ultrasmall N-doped MoS 2 nanocrystals (N-MoS 2 /CN) is fabricated by a selftemplating strategy, which realizes synergistically structural and electronic modulations of MoS 2 edges. Experiments and density functional theory calculations demonstrate that the N dopants could activate MoS 2 edges for HER, while the porous carbon network could deliver high accessibility of the active sites from N-MoS 2 nanocrystals. Consequently, N-MoS 2 /CN possesses superior HER activity with an overpotential of 114 mV at 10 mA cm −2 and excellent stability over 10 h, delivering one of best MoS 2based HER electrocatalysts. Moreover, this study opens a new venue for optimizing materials with enhanced accessible catalytic sites for energy-related applications.

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VS2 monolayers exhibit promising electrochemical properties for Li-, K-, and Mg-ion batteries.