 Highlights the B and N dual-dope carbon layer that encapsulated on MO2C nanocrystals MO2C at B and C were fabricated for accelerating her under alkaline condition. Theoretical calculations reveal that the H2O could be decomposed spontaneously over the introduced B sites and the defective C atoms in the dual-dope carbon layer provide the best H binding sites. The optimized dual-doped MO2C catalyst with synergistic effect of non-metal sites delivers superior her performances. This article was authored by Min Zhou, Shaoli Zhang, Wei Jikong, and others.