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Designing efficient electrode materials is necessary for supercapacitors but remains highly challenging. Herein, cobalt sulfide with crystalline/amorphous heterophase (denoted as Co(Al)S) derived from an Al metal–organic framework was constructed by ion exchange/acid etching and subsequent sulfidation strategy. It was found that rational sulfidation by adjusting the sulfur source concentration to a suitable level was favorable to form a 3D nanosheet-interconnected network architecture with a large specific surface area, which promoted ion/electron transport and charge separation. Benefiting from the features of the unique network structure and heterophase accompanied by aluminum, nitrogen and carbon coordinated in amorphous phase, the optimal Co(Al)S₍₁₀₎ exhibited a high specific capacity (1791.8 C g⁻¹ at 1 A g⁻¹), an outstanding rate capability and an excellent cycling stability. Furthermore, the as-assembled Co(Al)S//AC device afforded an energy density of 72.3 Wh kg⁻¹ at a power density of 750 W kg⁻¹, verifying that the Co(Al)S was a promising material for energy storage devices. The developed scheme is expected to promote the application of MOF-derived electrode materials in electrochemical energy storage and conversion fields.