To find out the better crosslinking monomer for vulcanization of natural rubber under electron beam (EB) radiation, the dry rubber was masticated with different polyfunctional monomers like TMPTA, NVP, and ethylene glycol diacrylate of different numbers of CH2- CH2-O group, such as 1G, 3G, 7G, and 10G. The masticated films were irradiated with different doses under EB at 10 kGy/pass. The highest tensile strength (25 MPa) of the rubber was observed in the presence of TMPTA (3phr) at 150 kGy dose. The gel content of the rubber increased with an increase of dose. Bionolle was mixed with the masticated rubber containing 3 phr TMPTA at different proportions; films of these blends along with Bionolle were irradiated under EB with different doses. The concentration of rubber in Bionolle and radiation dose were optimized. The elastomer with 5% masticated showed the highest tensile strength (62 MPa). The gel content of the blends was found to increase with an increase of radiation dose as well as rubber concentration in Bionolle. The elastomers or blends were found to possess good thermal properties. The elastomers exhibited a much lower loss of tensile strength due to the thermal aging compared with pure Bionolle. The elastomers sustained their original shape for 300 min at 180 degreesC, whereas Bionolle sustained its shape for only 3 min at 120 degreesC under the same load (50 g). Among all the elastomers, 5% rubber containing elastomer was found to be better in all respects. It was observed from scanning electron microscopy and differential scanning calorimetry studies that 5% rubber is well mixed with Bionolle.