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To reduce the charge‐transfer resistance of supercapacitors and achieve faster reversible redox reactions, ternary Ni‐Co‐Fe layered double hydroxide was prepared by using the urea method and then calcined to give NiCoFe oxide (NiCoFeO). To enhance conductivity, a polyaniline (PANI) conductive layer was assembled on the surface of the NiCoFeO particles by in situ oxidative polymerization of aniline monomers. The as‐prepared NiCoFeO/PANI composite was successful employed as a supercapacitor electrode. It was found that the NiCoFeO/PANI composite displayed good cycling stability, with a capacity loss of only 29.54 % after 5000 cycles. Furthermore, the NiCoFeO/PANI composite also exhibited excellent supercapacitor performance, with a high specific capacity of 843 F g−1 at a current density of 2 A g−1, whereas NiCoFeO showed a specific capacity of only 478 F g−1. This result was attributed to the synergistic effect between NiCoFeO and PANI. The facile synthesis strategy and excellent electrochemical performance suggest that NiCoFeO/PANI is a promising economical electrode material for applications in supercapacitors. Composites for supercapacitors: A novel NiCoFeO/polyaniline (PANI) composite was fabricated by in‐situ oxidative polymerization and applied as an electrode material for supercapacitors. The composite displayed excellent supercapacitor performance with a high specific capacity of 843 F g−1 at a current density of 2 A g−1 and good cycling stability, with a capacity loss of only 29.54 % after 5000 cycles (see figure). [ABSTRACT FROM AUTHOR]