This study presents an in situ growth technique to develop highly sensitive plasmonic fiber optic sensors with an excellent control over the plasmonic properties of gold (AuNPs) and silver nanoparticles (AgNPs). Here, we exploit the dual functionality of the U-bent fiber optic sensor (FOS) probes, where the probe acts as, firstly, the substrate for nanoparticles’ growth and, secondly, an invaluable tool to monitor as well as control the gold and silver seed binding to the surface amine groups and subsequently their growth in real time by means of the evanescent wave absorbance (EWA) spectral response. Au and Ag seeds (< 5 nm) with a peak absorbance at 510 and 390 nm, respectively, were used. The NP growth kinetics from the probes for different seed densities with a peak EWA response of 0.05, 0.1, and 0.15 optical density (OD) were observed in the presence of the respective metal precursor, cetyltrimethylammonium bromide (CTAB), and ascorbic acid. In comparison with AuNP grown FOS, a significant anisotropic growth was observed for AgNP with a redshift and spectral width as high as 215 nm and 425 nm, respectively, for a peak EWA response of 2.0 OD. The localized surface plasmon resonance (LSPR) activity of the AuNPs and AgNP grown FOS probes was evaluated for seed density of 0.1 OD. These proof-of-the-concept studies show significantly high RI sensitivity and surface-enhanced Raman scattering (SERS) enhancement factor for AgNP probes at 15.8 ΔA/RIU (for 22 AgNPs/μm2) and 1.3 × 107, respectively, in comparison with 18.9 ΔA/RIU (for 1424 AuNPs/μm2) and 1.1 × 106, respectively, for AuNP FOS probes. In addition, these plasmonic probes were stable in organic solvent (hexane) but its stability was deteriorated in alkaline solution (1 M NaOH).