Although transition metal phospho-sulfides deliver outstanding electrochemical performance, complex preparation methods hindered their further development. Herein, we report a facile one-step electrodeposition approach to deposit interconnected nanowalls-like nickel cobalt phospho-sulfide (Ni-Co-P-S) nanosheets onto the surface of carbon cloth. The thin Ni-Co-P-S nanosheets with multi-components and synergetic effects delivered rich active sites, further enhancing reversible capacitance. Therefore, the as-prepared Ni-Co-P-S electrode materials exhibit excellent electrochemical performance in a three-electrode system, showcasing a high specific capacitance of 2744 F/g at 4 A/g. The full supercapacitors based on Ni-Co-P-S as positive electrode and active carbon as negative electrode showcase a high specific capacitance of 110.9 F/g at 1 A/g, impressive energy density of 39.4 Wh/kg at a power density of 797.5 W/kg in terms of excellent cycling stability (91.87% retention after 10,000 cycles). This simple electrode position strategy for synthesizing Ni-Co-P-S can be extended to prepare electrode materials for various sustainable electrochemical energy storage/conversion technologies.