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Herein, we present a new method to construct a graphene wrapped yolk–double shell NiGa2S4 hollow microsphere (GW@YDSNGSHM) as a cathode electrode and a graphene wrapped FeS2–FeSe2 core–shell cratered sphere (GW-FeS2–FeSe2-CSS) as an anode electrode to enhance the performance of asymmetric supercapacitors. The GW@YDSNGSHM electrode shows considerable improvement of electrochemical performance including small internal resistance, reversibility, rapid kinetics, exceptional durability, and a notable specific capacitance (SC) of 2868.4 F g−1. The advancement in the performance of the GW-FeS2–FeSe2-CSS includes a good SC of 634.6 F g−1 and preferable durability. An asymmetric supercapacitor composed of the GW@YDSNGSHM (cathode) and GW-FeS2–FeSe2-CSS (anode) was assembled and tested. The advanced device revealed a SC of 352.30 F g−1 and an energy …