The commercial application of biodegradable metals (BMs), such as iron (Fe) and zinc (Zn), is hampered by their slow degradation rate. Polylactide (PLA) coatings on BMs have been proven to accelerate the corrosion of Fe and Zn but with limited success. This is the first study exploring the use of gold nanoparticles (Au NPs) to enhance and control the corrosion of polylactide (PLA)-coated Fe and Zn. The Au NPs enhanced the corrosion rate of Fe and Zn by promoting micro-galvanic corrosion after nanoparticle agglomeration. The optimal corrosion acceleration depended on the polymer's molecular weight, coating thickness, and coating structure. The results suggest that the Au-reinforced PLA-based coatings can be used to control Fe and Zn corrosion rates in the physiological environment.