Sol-gel synthesized La(1-x)SrxMnO3–BaTiO3 nanocomposites with varying strontium content were investigated to explore the influence of Sr doping on their properties. X-ray diffraction confirmed the perovskite phase purity. Sr doping resulted in a tunable bandgap, widening from 2.33 eV to 2.57 eV as Sr content increased, as revealed by Diffuse Reflectance Spectroscopy. Vibrating Sample Magnetometry measurements exhibited a Sr-dependent decrease in saturation magnetization (22 emu/g for x = 0.2 to 14 emu/g for x = 0.5). Dielectric analysis demonstrated an enhanced dielectric constant and the emergence of new relaxation behaviors with Sr doping. These findings unveil the tailorable optical, magnetic, and dielectric properties of LSMO-BTO nanocomposites due to Sr doping, suggesting their potential for diverse technological applications.