Ag/TiO2 nanocomposite films were successfully fabricated via a controllable magnetron sputtering strategy by regulating Ag sputtering power. Z-scan measurements under 515-nm laser excitation demonstrated that the composites significantly enhanced the nonlinear optical (NLO) performance of TiO2. Among them, the 9W-Ag/TiO2 sample exhibited the optimal performance, with its nonlinear absorption coefficient (β) and nonlinear refractive coefficient (n2) reaching 3.41 and 3.84 times those of pure TiO2, respectively. The core mechanism underlying the NLO performance enhancement lies in the synergy of multiple effects: Ag nanoparticles induce surface plasmon resonance (SPR) to amplify the localized light field; the work function difference between Ag and TiO2 facilitates the directional transfer of excited carriers at the interface, and meanwhile, interfacial localized strain further modulates charge distribution and improves carrier separation efficiency, collectively optimizing the NLO response of TiO2. This study provides a theoretical basis and experimental paradigm for the structural design and performance tuning of noble metal/transition metal oxide (TMO) composite NLO materials, while laying the foundation for their practical application in integrated optoelectronic devices such as optical limiters and ultrafast modulators.