Transition metal diborides represented by MoB2 have attracted widespread attention for their excellent acidic hydrogen evolution reaction (HER). Nevertheless, their electrocatalytic performance is generally unsatisfactory in high-pH electrolytes. Heterogeneous interface engineering is one of the most promising methods for optimizing the composition and structure of electrocatalysts, thereby greatly affecting their electrochemical performance. Herein, a heterostructure, composed of MoB2 and carbon nanotubes (CNTs), is rationally constructed by boronizing precursors including (NH4 )4 [NiH6 Mo6 O24 ]·5H2 O (NiMo6 ) and Co complexes on the carbon cloth (Co,Ni-MoB2 @CNT/CC). In this method, NiMo6 is boronized to form MoB2 by a modified molten-salt-assisted borothermal reduction. Meanwhile, Co catalyzes extra carbon sources to grow CNTs on the surface of MoB2 . Thanks to the successful production of the heterostructure, Co,Ni-MoB2 @CNT/CC exhibits remarkable HER performance with a low overpotential of 98.6, 113.0, and 73.9mV at 10mAcm-2 in acidic, neutral, and alkaline electrolytes, respectively. Notably, even at 500mAcm-2 , the electrochemical activity of Co,Ni-MoB2 @CNT/CC exceeds that of Pt/C/CC in an alkaline solution and maintains over 50h. Theoretical calculations reveal that the construction of theheterostructure is beneficial to both water dissociation and reactive intermediate adsorption, resulting in superior alkaline HER performance.