Metal selenides exhibit great potential in energy storage systems owing to their diversified species, large interlayer spaces, and high theoretical specific capacity according to multiple ion-storage behaviors. In this work, heterostructured CoSe 2 / NiSe 2 coupled with sp 3 bonded N-doped carbon coating layers and interconnected with sp 2 bonded carbon nanotubes is synthesized through a room-temperature wet-chemistry approach and a selenization route with Co−Ni Prussian blue analogues as the precursor. The hybrid exhibits enhanced energy storage properties when utilized as an anode material for sodium-and potassium-ion batteries. The excellent performance of the hybrid can be indexed to the delicately design of the CoSe 2 /NiSe 2 heterostructure and the hybridization of it with sp 2 and sp 3 bonded carbonaceous materials synchronously. Experimental and theoretical calculation results demonstrate the heterostructure is constructed to acquire charge transfer driving forces to boost internal reaction dynamics. And there is a combination of the dual advantages of sp 3 and sp 2 bonded carbon, possessing not only the exceptional mechanics buffer capability of N-doped carbon coating layers but also the excellent electrical characteristics of carbon nanotubes to promote external reaction dynamics. In addition, to elucidate the differential sodium/potassium storage capability of the hybrid, theoretical calculations are further performed to indagate the adsorption energy of sodium and potassium on the CoSe 2 /NiSe 2 heterointerface by establishing five Na/K adsorption sites. The research provides an effective strategy for the melioration of internal/external reaction dynamics to deliver ions durably and efficiently in energy storage regions.