The controlled deposition of nanoparticles onto 3-D nanostructured films is still facing challenges due to the uncontrolled aggregation of colloidal nanoparticles. In the context of this study, a simple yet effective approach is demonstrated to decorate the silver nanoparticles (AgNP) onto the 3-D and anisotropic gold nanorod arrays (GNAs) through a bioinspired polydopamine (PDOP) coating to fabricate surface-enhanced Raman spectroscopy (SERS) platforms. Since the Raman reporter molecules (methylene blue, MB, 10 mu M) were not adsorbed directly on the surface of the plasmonic material, a remarkable decrease in SERS signals was detected for the PDOP-coated GNAs (GNA@PDOP) platforms. However, after uniform and well-controlled AgNP decoration on the GNA@PDOP (GNA@PDOP@AgNP), huge enhancement was observed in SERS signals from the resultant platform due to the synergistic action which originated from the interaction of GNAs and AgNPs. I also detected that PDOP deposition time (i.e., PDOP film thickness) is the dominant parameter that determines the SERS activity of the final system and 30 min of PDOP deposition time (i.e., 3 nm of PDOP thickness) is the optimum value to obtain the highest SERS signal. To test the reproducibility of GNA@PDOP@AgNP platforms, relative standard deviation (RSD) values for the characteristic peaks of MB were found to be less than 0.17, demonstrating the acceptable reproducibility all over the proposed platform. This report suggests that GNA@PDOP@AgNP system may be used as a robust platform for practical SERS applications.