Biocompatible optical fibers and waveguides are gaining attention as promising platforms for implantable biophotonic devices. Recently, the distinct properties of silk fibroin were extensively explored because of its unique advantages, including flexibility, process compatibility, long-term biosafety, and controllable biodegradability for in vitro and in vivo biomedical applications. In this study, we developed a novel silk fiber for a sensitive optical sensor based on surface-enhanced Raman spectroscopy (SERS). In contrast to conventional plasmonic nanostructures, which employ expensive and time-consuming fabrication processes, gold nanoparticles were uniformly patterned on the top surface of the fiber employing a simple and cost-effective convective self-assembly technique. The fabricated silk fiber-optic SERS probe presented a good performance in terms of detection limit, sensitivity, and linearity. In particular, the uniform pattern of gold nanoparticles contributed to a highly linear sensing feature compared to the commercial multi-mode fiber sample with an irregular and aggregated distribution of gold nanoparticles. Through further optimization, silk-based fiber-optic probes can function as useful tools for highly sensitive, cost-effective, and easily tailored biophotonic platforms, thereby offering new capabilities for future implantable SERS devices.