Surface-enhanced Raman scattering (SERS) vastly improves signal-to-noise ratios as compared to traditional Raman scattering, making sensitive assays based upon Raman scattering a reality. However, preparation of highly stable SERS-active gold substrates requires complicated and expensive methodologies and instrumentation. Here, a general and completely solution-phase, seed-based approach is introduced, which is capable of producing gold films for SERS applications on a variety of substrates, not requiring surface modification or functionalization. SERS enhancement factors of ≈107 were observed. Moreover, solution-phase gold film deposition on highly complex surfaces, such as protein-coated bioassays, is demonstrated for the first time. Protein bioassays coated with such SERS-active gold films are combined with bioconjugated single-walled carbon nanotube Raman labels, affording highly sensitive detection of the cancer biomarker, carcinoembryonic antigen in serum, with a limit of detection of ≈5 fM (1 pg mL−1).