Vanadium redox flow batteries (VRFBs) have emerged as a promising energy storage solution for stabilizing power grids integrated with renewable energy sources. In this study, we synthesized and evaluated a series of zeolitic imidazolate framework-67 (ZIF-67) derivatives as electrode materials for VRFBs, aiming to enhance electrochemical performance. Four materials—Co/NC-700, Co/NC-800, Co3O4-350, and Co3O4-450—were prepared through thermal decomposition under different conditions and coated onto graphite felt (GF) electrodes. X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) analyses confirmed the structural integrity and distribution of the active materials. Electrochemical evaluations revealed that electrodes with ZIF-67-derived coatings exhibited significantly lower charge transfer resistance (Rct) and higher energy efficiency (EE) compared to uncoated GF electrodes. Co/NC-800//GF delivered the highest energy efficiency and discharge capacity among the tested configurations, maintaining stable performance over 100 charge–discharge cycles. These results indicate that Co/NC-800 holds great potential for use in VRFBs due to its superior electrochemical activity, stability, and scalability.