Exploring nonprecious electrocatalysts for water splitting with high efficiency and durability is critically important.Herein,bimetallic phosphides are encapsulated into graphitized carbon to construct a C@NiCoP composite nanoarray using bimetallic metal-organic framework (MOF) as a self-sacrificial tem-plate.The resulting C@NiCoP exhibits superior performance for pH-universal electrocatalytic hydrogen evolution reaction (HER),particularly representing a low overpotential of 46.3 mV at 10 mA cm-2 and Tafel slope of 44.1 mV dec-1 in alkaline media.The structural characterizations combined with theoret-ical calculation demonstrate that tailored electronic structure from bimetal atoms and the synergistic effect with graphitized carbon layer could jointly optimize the adsorption ability of hydrogen on active sites in HER process,and enhance the electrical conductivity as well.In addition,the carbon layer served as a protecting shell also prevents highly dispersed NiCoP components from agglomeration and/or loss in harsh media,finally improving the durability.This work thus provides a new insight into optimizing activity and stability of pH-universal electrocatalysts by the nanostructural design and electronic struc-ture modulation.