Surface-enhanced Raman scattering (SERS) is a powerful analysis technique that allows both the identification and detection of analytes at trace levels. However, the low rate of charge transfer (CT) between noble-metal nanoparticles and several analytes prevents them from being effectively detected by SERS-based sensors. They are regarded as low Raman crosssection molecules. In this study, we enhanced the performance of the silver nanoparticles (AgNPs)-based SERS sensing platform for a low Raman cross-section molecule, urea, focusing on improving the rate of CT. First, a set of Ag/titanium dioxide (TiO 2 ) nanocomposites were synthesized. The presence of TiO 2 improved the intensity of the SERS signal of urea, in comparison to the use of bare AgNPs. Second, a photoinduced enhanced Raman spectroscopy (PIERS) technique was employed to further elevate the Raman signal of urea. Thanks to the step of preirradiation using UV light at λ = 365 nm, with the use of the substrates containing 25%, 33%, and 50% TiO 2 content, enhancements of 1.93, 3.42, and 7.45 times were achieved, respectively, compared to the use of Ag/TiO 2 composites without UV irradiation. Through modification of the substrate, combined with application of the PIERS technique, the SERS system for urea detection using Ag/3TiO 2 (50% TiO 2 ) achieved a competitive detection limit of 4.6 × 10 −6 M. It also allowed the detection of urea in milk at concentrations down to 10 −5 M. This substrate modification and PIERS technique are promising for improvement of the sensing performance of other low-cross-section molecules.