Polycrystalline diamond compact (PDC) is a widely used superhard material, and its thermal stability and wear resistance are the main factors determining its performance. The residual cobalt binder content in polycrystalline diamond (PCD) has a significant impact on the thermal stability and wear resistance of PDC. Therefore, cobalt removal treatment is required to improve the performance of PDC. The current cobalt removal methods mainly include acid leaching and electrolysis. This study proposes a novel coupling method that combines acid leaching and electrolysis for cobalt removal. Cobalt removal was conducted for 10 h under the conditions of electrolytic voltage of 12 V, direct current power supply current of 0.01 A, and sulfuric acid electrolyte concentration of 9.2 mol/L. The cobalt removal effect was evaluated using scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), and X-ray diffraction (XRD). The hardness and elastic modulus of PDC before and after cobalt removal were measured using nanoindentation experiments. The results indicate that the coupled electrolysis process effectively removes the cobalt phase in the PCD layer while retaining the WC phase. The hardness and elastic modulus of PDC decrease after the removal of cobalt binder, and the cobalt removal depth can reach 807 μm.