Natural polymers have attracted a lot of interest in researchers of late as they are environmentally friendly, biocompatible, and possess excellent characters. Membranes forming natural polymers have provided a whole new dimension to the separation technology. In this work, chitosan-gelatin blend membranes were fabricated using chitosan as the base and varying the amount of gelatin. Transport, mechanical, and surface characteristics of the fabricated membranes were examined in detail by means of the characterizing techniques such as Fourier transform infrared spectroscopy, differential scanning colorimetry, wide angle X-ray diffraction, scanning electron microscope, and thermogravimetric analysis. In order to analyze the water affinity of the developed blend chitosan-gelatin membranes, the percentage degree of swelling was examined. Out of the fabricated membranes, the membrane loaded with 15 mass% of gelatin exhibited the better pervaporation performance with a pervaporation separation index value of 266 at 30 °C for the solution containing 10% in terms of the mass of water, which is the highest among the contemporary membranes. All the fabricated membranes were stable during the pervaporation experiments, and permeation flux of water for the fabricated membranes was dominant in the overall total permeation flux, signifying that the developed membranes could be chosen for efficient separation of water–isopropanol mixture on a larger scale.