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CoTe 2 -NiTe 2 heterojunction embedded inside and outside the mesoporous walls of nitrogen-doped carbon nanoboxes via a straightforward ZIF67-involved etching-anchoring-tellurization strategy (H-CoTe 2 /NiTe 2 @NCBs). The establishment of CoTe 2 /NiTe 2 heterojunction can effectively modulate the electronic reconfiguration at the interface, optimize the reaction pathways, and lower the energy barriers, thus affording an excellent electrocatalytic bifunctionality toward ORR and OER. [Display omitted] • CoTe 2 /NiTe 2 embedded in N-doped carbon nanoboxes are constructed. • The heterojunctions cause the spontaneous charge redistribution at the interfaces. • The H-CoTe 2 /NiTe 2 @NCBs creates abundant active sites and mass transfer pathways. • Due to synergistic effect, ORR and OER activities are significantly increased. • The Zn-air battery delivers high energy output and excellent cyclability. Interface engineering has been recognized as one of the most promising strategies for tuning the catalytic properties of catalysts. However, building well-defined nanointerfaces for efficient oxygen reduction/evolution reactions (ORR/OER) remains a challenge. Herein, a hollow heterostructure composed of highly-dispersed CoTe 2 inside the mesoporous walls of nitrogen-doped carbon nanoboxes and uniformly-dispersed NiTe 2 outside the mesoporous walls (H-CoTe 2 /NiTe 2 @NCBs) is designed via a ZIF67-involved etching-anchoring-tellurization strategy. Promising half-wave potential of 0.86 V and overpotential of 320 mV at 10 mA cm−2 are obtained by H-CoTe 2 /NiTe 2 @NCBs. The excellent ORR/OER activity of H-CoTe 2 /NiTe 2 @NCBs is ascribed to the synergistic coupling based on nanointerfaces between CoTe 2 and NiTe 2. Density functional theory calculations confirm that the nanointerface-based electronic coupling between CoTe 2 and NiTe 2 facilitates the charge transfer between two components and generates abundant catalytically active sites at the heterointerface, thereby significantly promoting the ORR/OER activities. This work provides the design principles for transitional bimetallic tellurides as bifunctional electrocatalysts. [ABSTRACT FROM AUTHOR]