Development of high performance anode materials is of critical importance for advanced lithium-ion batteries. Herein, we report a novel 3D hybrid composed of well-dispersed Co2P nanoparticles embedded in N-doped carbon nanotubes grown on porous carbon polyhedral (Co2P/NCNTFs) as advanced electrode for lithium-ion batteries. The Co2P/NCNTF electrode is synthesized with a facile pyrolysis and phosphidation method derived from a cobalt-based zeolitic imidazolate framework. The resultant Co2P/NCNTFs hybrid demonstrates superior electrochemical performance in lithium-ion batteries, with a large discharge capacity of 906 mA h g(-1) at 100 mA g(-1), excellent rate performance of 508 mA h g(-1) at 6.4 A g(-1), high Coulombic efficiency of 99.4% after 300 cycles at 100 mA g(-1), and high cycling performance with a capacity retention of 94.7%, which is among the best obtained results for Co2P-based anode materials.