Vacancies have received considerable attention in energy storage materials since they are able to generate more active defects, leading to enhanced conductivity and thus higher capability. Here, we provide a facile strategy to rapidly achieve sufficient sulphur vacancies, lattice distortion and changed charge-states of Ni/Co on the material surface layer in NiCo2S4via low-temperature atmospheric pressure plasma. Both experimental results and DFT calculations have demonstrated that enhanced performances can be obtained with different amounts of sulphur vacancies (S-vacancies), with optimal performance obtained at 30% S-vacancy. Moreover, the same trend of enhanced energy storage performance effects is found in comparison groups of varied Ni/Co atomic ratios (1 : 1, 2 : 1, 1 : 4, 4 : 1), suggesting the serviceability of this facile strategy, which only requires 30 seconds of processing. This paves a path towards high-performance supercapatteries using the simple plasma-based method.