This paper deals with the development of compatible blend membranes of chitosan (CS) and gelatin (GL) by solution casting and crosslinking with glutaraldehyde. The membranes were tested in pervaporation (PV) dehydration of 1,4-dioxane. Membrane characterizations by Fourier transform infrared spectroscopy, wide-angle X-ray diffraction, and a universal testing machine were done to understand their physicochemical properties and for their suitability under PV conditions. The blend membranes were more water selective compared to pristine chitosan membrane at 30 degrees C. Flux increased with increasing wt.% of water of the feed and also by increasing the gelatin content of the blend, but selectivity decreased. Sorption experiments gave information on the interaction between feed mixture and membrane polymers. Membranes of this study could extract nearly 97wt.% of water from the feed mixture. Arrhenius activation parameters and diffusion coefficients estimated from a temperature dependence of PV results could explain the PV results satisfactorily.