Localized surface plasmonic resonance (LSPR) biosensing using optical fibers has gained popularity due to its label-free approach and high sensitivity to changes in the nanoparticle surface's local index of refraction. However, improving sensitivity remains a challenge. In this study, a two-step approach was employed to fabricate a composite structure using gold nanoparticles and monolayer graphene (Gr-AuNPs). The combination of AuNPs and graphene membrane demonstrated high potential for Surface-enhanced Raman scattering (SERS) and surface plasmonic resonance (SPR) fiber sensors. The Gr-AuNPs sensor successfully detected R6G molecules with a low detection limit of 10−12 M, indicating promising SERS activity. Numerical simulations confirmed that the graphene generated densely hot spots in the nanogap region between plasmonic layers. It's interesting that the proposed SPR-SERS Sensor can detect both glucose and thiram. This demonstrates the sensors practicality and can help with a basic environmental need to find leftover pesticides in the soil. The combination of SPR-SERS dual-mode detection provides more options for detecting and verifying data, increasing the precision and repeatability of experiments.