Limited by the intrinsic semiconductor behavior and the number of active sites, the application of MoS 2 as an electrocatalyst is hindered. Doping is an easiest strategy to improve its properties. In addition, it is found that the interlayer-regulatory can be used as another strategy to improve the catalytic properties of MoS 2 . Therefore, we apply the first-principles method to systematically study the effect of interlayer doping on the catalytic properties of MoS 2 disulfide. Furthermore, we investigate the influence of the interlayer-doped systems on the catalytic hydrogen evolution of MoS 2 . The results show that the interlayer doping strengthens the interaction between the monolayer of MoS 2 , which is beneficial to improve the structural stability. Importantly, interlayer doping promotes local hybridization at the Fermi level inducing the interlayer-doped MoS 2 to show a degree of metallic behavior. As a result, it is obviously beneficial to improve the catalytic hydrogen evolution effect of MoS 2 . Finally, it is found that hydrogenated C-doped MoS 2 , with excellent geometric and structural stability, shows the best catalytic hydrogen evolution effect because the weak local hybridization of C-2p at the Fermi level weakens the interaction between Mo and S.