It is extremely crucial to design and match high‐quality cathode and anode for achieving high‐performance asymmetric supercapacitors (ASCs). Herein, Co3(PO4)2@NiCo‐LDH/Ni foam (CP@NCOH/NF) cathode with hierarchical morphology and graphene hydrogel/Fe–Ni phosphide/Ni foam (GH/FNP/NF) anode with the robust and porous structure are elaborately designed and prepared, respectively. Owing to their unique and profitable structures, both CP@NCOH/NF and GH/FNP/NF electrodes yield the superior capacity (10760 and 2236 mC cm−2 at 2 mA cm−2, respectively), good rate capability (63% retention at 200 mA cm−2 and 52% retention at 50 mA cm−2, respectively), and excellent cycling stability (72% and 74% retention after 10 000 cycles, respectively). Benefiting from their matchable electrochemical performances, the configured solid‐state CP@NCOH/NF//GH/FNP/NF ASC outputs both competitive energy density (80.2 Wh kg−1/4.1 mWh cm−3) and power density (14563 W kg−1/750 mW cm−3), companied by remarkable cyclability (71% retention after 10 000 cycles), manifesting its great promise for large‐scale integrated energy‐storage system.