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• Co 3 V 2 O 8 -T (T = temperature/°C) are prepared as bifunctional electrocatalysts. • Co 3 V 2 O 8 -400 nanofibers show small Tafel slopes of 43 and 63 mV dec−1 for ORR and OER. • The Co 3 V 2 O 8 -400 nanofiber has the best catalytic activities for ORR and OER. • The mechanism of Co 3 V 2 O 8 -400 nanofiber is simulated by DFT. Highly active and stable bifunctional electrocatalysts towards oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are necessary for practical fuel cells, metal-air batteries, and water splitting. Herein, we report a series of bifunctional Co 3 V 2 O 8 -T (T = temperature/°C) electrocatalysts by using Co-carbon electrospun nanofiber as a template, followed by a one-step calcination process. As expected, the developed Co 3 V 2 O 8 -400 nanofiber electrocatalyst shows a very small Tafel slope of 43 and 63 mV dec−1 for the ORR and OER in the alkaline solution, respectively. In addition, density functional theory (DFT) calculations reveal that the metallic conductivity and interface V-Co interaction of Co 3 V 2 O 8 -400 nanofiber boost ORR and OER electrocatalytic reactions. [ABSTRACT FROM AUTHOR]