Constructing active heterointerfaces is powerful to enhance the electrochemical performances of transition metal dichalcogenides, but the interface density regulation remains a huge challenge. Herein, MoO 2 /MoS 2 heterogeneous nanorods are encapsulated in nitrogen and sulfur co-doped carbon matrix (MoO 2 /MoS 2 @NSC) by controllable sulfidation. MoO 2 and MoS 2 are coupled intimately at atomic level, forming the MoO 2 /MoS 2 heterointerfaces with different distribution density. Strong electronic interactions are triggered at these MoO 2 /MoS 2 heterointerfaces for enhancing electron transfer. In alkaline media, the optimal material exhibits outstanding hydrogen evolution reaction (HER) performances that significantly surpass carbon-covered MoS 2 nanorods counterpart (η 10 : 156 mV vs 232 mV) and most of the MoS 2 -based heterostructures reported recently. First-principles calculation deciphers that MoO 2 /MoS 2 heterointerfaces greatly promote water dissociation and hydrogen atom adsorption via the O-Mo-S electronic bridges during HER process. Moreover, benefited from the high pseudocapacitance contribution, abundant "ion reservoir"-like channels, and low Na + diffusion barrier appended by high-density MoO 2 /MoS 2 heterointerfaces, the material delivers high specific capacity of 888 mAh g −1 , remarkable rate capability and cycling stability of 390 cycles at 0.1 A g −1 as the anode of sodium ion battery. This work will undoubtedly light the way of interface density engineering for highperformance electrochemical energy conversion and storage systems.