Layered double hydroxides (LDHs) and metal sulfides (MSs) have been widely used as promising electrode materials for supercapacitors, and the rational architectural design of MS/LDH heterogeneous structures is critical to optimize large energy storage. Herein, a precisely designed hollow Co₉S₈ nanotubes@CoNi-LDH nanosheet heterostructure on Ni foam, facilely prepared by an ingenious in situ strategy in this Co₉S₈ nanoarray was first used as the self-sacrificing template and metal source to in situ synthesize Co-ZIF-67 polyhedron to form the Co₉S₈@ZIF-67 heterostructure, and then Co₉S₈@ZIF-67 was in situ etched successfully using Ni²⁺ ions to form the final Co₉S₈@CoNi-LDH/NF core–shell nanoarray. This in situ synthetic strategy to fabricate the heterostructure is conducive to boosting the structural stability, modifying the electric structure and regulating the interfacial charge transfer. Due to the synergistic effect and tight heterogeneous interface, Co₉S₈@CoNi-LDH/NF displayed an outstanding capacitance of 9.65 F cm⁻² at a current density of 2 mA cm⁻² and excellent capacitance retention rate of 91.7% after 5000 cycles. In addition, the ASC device assembled with AC has an extremely high energy density of 1.0 mW h cm⁻² at 2 mA cm⁻² and maintains 96.9% capacitance retention after 5000 cycles. This work provides a skillful strategy for the precise design and in situ synthesis of MS/LDH heterostructures with fascinating features for electrochemical energy storage applications.