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Flexible yolk-shelled NiCo2S4 hollow spheres/reduced graphene oxide (RGO) hybrid lamellar films were successfully fabricated by developing a facile strategy of vacuum filtration. After constructing the sandwich-like structures, the NiCo2S4 hollow spheres were inserted in-between the RGO nanosheets, which effectively prevented the self-restacking of RGO nanosheets and increased the interlayer spacing, leading to fast ion penetration and diffusion. The as-prepared NiCo2S4/2RGO hybrid lamellar films with excellent conductivity delivered an appreciable capacitance of 1000.5 F g−1 at 1 A g−1. Moreover, an asymmetric supercapacitor (ASC) was successfully synthesized utilizing activated carbon (AC) and NiCo2S4/2RGO hybrid lamellar films as the negative electrode and positive electrode, which manifested a high energy density (15.4 W h kg−1) and power density (2227.3 W kg−1) coupled with remarkable cycling stability (80.5% retention over 5000 cycles). After charging, two ASC devices connected in series were capable of lighting two red LEDs connected in parallel for at least 2.0 minutes. [ABSTRACT FROM AUTHOR]