Ethylene vinyl acetate (EVA)/natural rubber (SMR L)/organoclay nanocomposites were prepared by melt blending technique with 0-10 phr organoclay loading and 3 phr TMPTA. Electron beam initiated crosslinking on these samples was carried out using a 3.0 MeV electron beam machine with doses ranging from 50 to 200 kGy. XRD results proved that dispersion of organoclay in the nanocomposites was slightly improved by irradiation with TMPTA. This was further supported by transmission electron microscopy images, where the nanoscale dispersion of organoclay was more homogenous throughout the irradiated polymer matrix compared to nonirradiated samples. TMPTA also increased the gel fraction yield, tensile properties and thermal stability of the irradiated neat EVA/SMR L and its nanocomposites. TMPTA was found to act as a crosslink initiator, which promotes crosslink bridges via free radical mechanism in EVA/SMR L matrix. SEM observation shows that the fracture behavior of the irradiated neat EVA/SMR L and its nanocomposites with TMPTA is significantly different compared to the fracture behavior of the nonirradiated neat EVA/SMR L. The distinct failure surface structure formed in the irradiated samples with TMPTA explains the overall higher value of tensile properties. (C) 2010 Wiley Periodicals, Inc. J Appl Polym Sci 117: 865-874, 2010