The large grain boundary resistance between different components of the anode electrode easily leads to the low ion transport efficiency and poor electrochemical performance of lithium-/sodium-ion batteries (LIBs/SIBs). To address the issue, a Janus heterointerface with a Mott−Schottky structure is proposed to optimize the interface atomic structure, weaken interatomic resistance, and improve ion transport kinetics. Herein, Janus Co/Co 2 P@carbon-nanotubes@core−shell (Janus Co/ Co 2 P@CNT-CS) refined urchin-like architecture derived from metal−organic frameworks is reported via a coating−phosphating process, where the Janus Co/Co 2 P heterointerface nanoparticles are confined in carbon nanotubes and a core−shell polyhedron. Such a Janus Co/Co 2 P heterointerface shows the strong built-in electric field, facilitating the controllable ion transport channels and the high ion transport efficiency. The Janus Co/Co 2 P@CNT-CS refined urchin-like architecture composed of a core−shell structure and the grafting carbon nanotubes enhances the structure stability and electronic conductivity. Benefiting from the spaced-confined Janus heterointerface engineering and synergistic effects between the core−shell structure and the grafting carbon nanotubes, the Janus Co/Co 2 P@CNT-CS refined urchin-like architecture demonstrates the fast ion transport rate and excellent pseudocapacitance performance for LIBs/SIBs. In this case, the Janus Co/ Co 2 P@CNT-CS refined urchin-like architecture shows high specific capacities of 709 mA h g −1 (200 cycles) and 203 mA h g −1 (300 cycles) at a current density of 500 mA g −1 for LIBs/SIBs, respectively.