• The critical bimetallic phosphide layer (CBPL) exhibits high electrical conductivity and forms heterostructures with NiCo-LDH, improving the electrical conductivity of the hybrid cathode (NiCo-P1.0).
• CBPL facilitates OH⁻ adsorption and synergizes with NiCo-LDH in electrode reactions, delivering extra energy.
• NiCo-P1.0 cathode delivers 286.64 mAh g⁻¹ at 1C with a retention of 72.22% at 40C, and the assembled NiCo-P1.0//Zn battery achieves energy density/power density of 503.62 Wh kg⁻¹/18.62 kW kg⁻¹.
• The flexible quasi-solid-state pouch cell maintains stable output after deformation, validating practicality.