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Tailoring hierarchical hybrid core-shell electrodes with impartial microstructural features and excellent electroactive constituents is crucial for the design of high-performance supercapacitors (SCs). Herein, for the first time, we fabricate uniformly aligned porous ZnFe2O4 (ZFO) nanosheet arrays onto reduced graphene oxide-garnished conductive Ni foam (rGO-NF) substrates and subsequently embellish the first layer of ZFO nanosheets with morphology-controlled secondary NiMoO4 nanosheets to achieve a hierarchical 3D core-shell structure