The rational exploration of hybrid materials with well-defined compositions and structures/morphologies is essential for achieving high-performance electrodes for supercapacitors. Here, in situ dispersion and anchoring of NiCoP nanoparticles (NPs) on a bimetal-organic framework (Co1Ni2-MOF) by a controllable partial phosphorization approach are reported. The phosphating temperature and time significantly affect the specific capacitance of NiCoP/Co1Ni2-MOF-X-Y (where X and Y represent the phosphating temperature and time, respectively). Co1Ni2-MOF provides anchoring sites for confining NiCoP NPs, effectively improving the stability of NiCoP NPs. Highly dispersed NiCoP NPs facilitate OH- adsorption, boosting the redox reaction kinetics. NiCoP/Co1Ni2-MOF-350-2 with optimized phosphating conditions exhibits a high specific capacitance of 525 F g-1 at 0.5 A g-1, which is superior to that of the precursor of Co1Ni2-MOF. Moreover, a hybrid supercapacitor constructed with NiCoP/Co1Ni2-MOF-350-2 and activated carbon shows a high specific capacitance and outstanding long-term stability.