The outstanding multifunctional electrochemical properties of chalcogenide-based FeO@CuCo2S4, such as electrochemical energy storage (EES) and electrocatalytic oxygen evolution reaction are demonstrated. The FeO@CuCo2S4 film is fabricated using a two-step synthesis procedure. First, CuCo2S4 was grown on 3D porous nickel foam substrate using a mild hydrothermal growth technique, onto which FeO was then deposited via a magnetron sputtering. The FeO@CuCo2S4 film shows a cordillera-like morphology with a uniformly distributed island-like nanospheres on its surface. The optimized FeO@CuCo2S4 electrode delivers an ultrahigh specific capacitance of 3213 F g(-1) at 1 A g(-1). This FeO@CuCo2S4 electrode shows superior capacity retention and coulombic efficiency of similar to 116% and similar to 99%, respectively, after 10 000 charge/discharge stability cycles. Moreover, this superior electrode is also serves as an OER electrocatalyst in alkaline solution (1 M aqueous KOH), demonstrating better catalytic activity by attaining a low overpotential of similar to 240 mV at 10 mA cm(-2) and a small Tafel slope of 51 mV dec(-1). This FeO@CuCo2S4 catalyst has excellent current rate performance and endurance properties at a high current density rate of up to 100 mA cm(-2) even after 25 hours. The post-measurement HR-TEM, EDS-STEM mapping, and Raman analysis reveal the phase transformation of FeO@CuCo2S4 upon electro-oxidation.