Metal-organosulfide coordination polymers (MOSCPs) are important functional materials with attractive application prospects. Herein a two-dimensional structural MOSCP was fabricated on nickel foam with nanosheet array morphology. When as the binder-free battery-type electrode for a supercapacitor, the as-prepared Co-based MOSCP showed high specific capacitance (759 F g(-1)/379.5 C g(-1)/105.4 mAh g(-1) at 0.5 A g(-1)), excellent rate performance (58.8% after the current density increased 20 times), and good cycle stability (73.4% after 5000 cycles). In addition, a maximum energy density of 31.97 Wh kg(-1) was obtained at a power density of 375.01 W kg(-1) in the assembled asymmetric supercapacitor device. These results indicated that this work would open up a new path to design and prepare the battery-type electrode for a supercapacitor by exploring nanoscale MOSCP materials.