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Transition metal phosphides/phosphates (TMPs) are considered appealing electrode materials in energy-related fields, especially in supercapacitors. However, the dilemma of inadequate electrode kinetics and dimensional unreliability evoked by a huge volume variation during cycling significantly plagues their progress. To mitigate this issue, in this work, a 3D cross-network in situ assembled via self-derived N-doped carbon hybrid Ni-Co-P/POx 2D sheets is fabricated. Particularly, high-Fermi-level N-doped carbon well confines Ni-Co-P/POx nanoparticles at the molecular level, and N-doping leads to redistribution of spin/electron density in the carbon skeleton, effectively regulating the electron environment of nearby Ni-Co-based moieties, resulting in a relatively lower surface work function, as known via experimental and Kelvin probe force microscopy (KPFM) results, which favors electron flee from the electrode surface and facilitates electron transport toward a rapid supercapacitor response. Moreover, the well-defined 3D cross-network architectures featured with in-plane pores and interconnected with each other can provide more ion/electron transfer pathways and 2D sheets with excellent surface chemistry available for sustainable ion/electron mobility, synergistically affording the favorable electrode kinetics. Accordingly, the resultant Ni-Co-P/POx@NC electrode shows admirable specific capacitance, excellent rate survivability, and long-term cyclability. The as-assembled asymmetric device exhibits remarkable energy and power outputs (48.5 Wh kg