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• Flake-like K 2 Co 3 (P 2 O 7) 2 ·2H 2 O (KCoPi) was prepared by a hydrothermal method. • The as-prepared KCoPi features a layered structure and zigzag chains of CoO 6. • The KCoPi nanoflakes exhibit remarkable OER activity in alkaline solution. Alkali metal cobalt phosphates show great potential as electrocatalysts for oxygen evolution reaction (OER). Herein, a kind of layered potassium cobalt pyrophosphate dehydrate, i.e., K 2 Co 3 (P 2 O 7) 2 ·2H 2 O, was prepared by a simple hydrothermal method, and was proved to be a novel OER electrocatalyst for the first time. The as-developed K 2 Co 3 (P 2 O 7) 2 ·2H 2 O features a layered structure, large specific surface area, and special zigzag CoO 6 octahedral chains, all of which contribute to the highly efficient OER performance. In specific, it achieves 10 mA cm−2 at an overpotential of only 296 mV and a Tafel slope of 40.2 mV dec−1 in 1.0 M KOH. Thus, this present work has opened a new pathway to develop alkali metal cobalt phosphates towards efficient and stable electrocatalytic oxygen evolution reaction. [ABSTRACT FROM AUTHOR]