We demonstrated a method to improve the output performance of a Ti:sapphire laser in the long-wavelength low-gain region with an efficient stimulated Raman scattering process. By shifting the wavelength of the high-gain-band Ti:sapphire laser to the long-wavelength low-gain region, high-performance Stokes operation was achieved in the original long-wavelength low-gain region of the Ti:sapphire laser. With the fundamental wavelength tuning from 870 to 930 nm, first-order Stokes output exceeding 2.5 W was obtained at 930–1000 nm, which was significantly higher than that directly generated by the Ti:sapphire laser, accompanied by better beam quality, shorter pulse duration and narrower linewidth. Under the pump power of 42.1 W, a maximum first-order Stokes power of 3.24 W was obtained at 960 nm, with a conversion efficiency of 7.7%. Furthermore, self-mode-locked modulations of first- and second-order Stokes generation were observed in Ti:sapphire intracavity solid Raman lasers for the first time.