Chitosan-sulfated titania composite membranes were prepared, characterized, and evaluated for potential application as polymer electrolyte membranes. To improve the chemical stability, the membranes were cross-linked using sulfuric acid, pentasodium triphosphate, and epoxy-terminated polydimethylsiloxane. Differences in membranes’ structure, thickness, morphology, mechanical, and thermal properties prior and after cross-linking reactions were evaluated. Membranes’ water uptake capacities and their chemical stability in Fenton reagent were also studied. As proved by dielectric spectroscopy, the conductivity strongly depends on cross-linker nature and on hydration state of membranes. The most encouraging results were obtained for the chitosan-sulfated titania membrane cross-linked with sulfuric acid. This hydrated membrane attained values of proton conductivity of 1.1 × 10−3 S/cm and 6.2 × 10−3 S/cm, as determined at 60 °C by dielectric spectroscopy and the four-probes method, respectively.