Graft copolymerization of nitrile monomers, such as acrylonitrile and methacrylonitrile, onto bleached sulfonated jute-cotton blended fabric was carried out in an aqueous medium using potassium permanganate as an initiator under the catalytic influence of sulfuric acid in a nitrogen atmosphere. The effect of concentrations of monomer, permanganate, sulfuric acid, reaction time, and reaction temperature on the percent graft yield was studied. The percent graft yield was found to be dependent on the abovementioned variables. On the basis of experimental findings, an optimum condition for effective grafting is suggested. As evidence of polymer grafting, some instrumental analyses, such as thermogravimetric analysis, infrared spectroscopy, and X-ray diffractometry were carried out. Grafting improved the thermal stability, protected from photo-oxidative degradation, affected dyeability, and had a positive impact on color fastness.