Polylactide (PLA) is a bio-based polymer due to its excellent biocompatibility, outstanding optical properties and sufficient tensile strength. However, PLA with a linear chain structure is inherent brittle therefore exhibit a poor ductility, restricting the use of PLA in large-scale applications. To improve the toughness of PLA, many soft polymers have been used, whereas its mechanical properties are restricted due to poor interfacial compatibility between the toughening and matrix phase. The electron-induced reactive processing (EIReP) is a novel method to modify the properties of polymers by inducing compatibilization chemical reactions without using additives. To fulfilled challenges in case environmentally friendly upcoming application, the development of sustainable high-performance composites which are biodegradable due to the use of 100% bio-based renewable polymer materials is a promising strategy. Therefore is it reasonable to employ a sustainable electron beam treatment instead of using the petroleum-based additives. In this study, the morphological, mechanical, and thermal properties of natural rubber (NR) modified PLA by electron beam (EB) treatment have been investigated. The induced free radicals initiating a competing chain scission and cross-linking reactions of the PLA material. Hence the PLA/NR blends were irradiated at optimal processing parameters with various dose values. The corresponding structure-morphology-property relationships of electron modified PLA blends have been thoroughly explored by many measurements such as the SEM, DSC DMA and rheology.