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By performing DFT computations, we proposed a promising strategy to tune the ORR/OER catalytic performance of transition metal-nitrogen-carbon by constructing heterostructure with graphdiyne. We found the d-band center and charge transfer of the TM active sites can correlate the ORR/OER catalytic activity and their electronic properties for TM N C/GDY. [Display omitted] • The catalytic activities of the heterostructure between TM N C with GDY (TM N C/GDY) for ORR/OER were studied by means of density functional theory. • Co N C/GDY can be proposed as a bifunctional catalyst for ORR/OER with low overpotential. • According to the constant-potential method, the acidic condition is conducive to boost bifunctional catalytic activity for Co N C/GDY. Exploring high-efficiency electrocatalysts to boost the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is pivotal to the large-scale applications for clean and renewable energy technologies, such as fuel cells, water splitting, and metal–air batteries. Herein, by means of density functional theory (DFT) computations, we proposed a strategy to modulate the catalytic activity of transition metal-nitrogen-carbon catalysts through their interface engineering with graphdiyne (TM N C/GDY). Our results revealed that these hybrid structures exhibit good stability and excellent electrical conductivity. Especially, Co N C/GDY was identified as a promising bifunctional catalyst for ORR/OER with rather low overpotentials in acidic conditions according to the constant-potential energy analysis. Moreover, the volcano plots were established to describe the activity trend of the ORR/OER on TM N C/GDY using the adsorption strength of the oxygenated intermediates. Remarkably, the d-band center and charge transfer of the TM active sites can be utilized to correlate the ORR/OER catalytic activity and their electronic properties. Our findings not only suggested an ideal bifunctional oxygen electrocatalyst, but also provided a useful strategy to obtain highly efficient catalysts by interface engineering of two-dimensional heterostructures. [ABSTRACT FROM AUTHOR]