Nylon 66 has been transformed into a material with significantly improved properties like hardness, tensile strength, and flexural modulus by processing it under the optimized dose rate of electron beam in the presence of suitable crosslinkers. Furthermore, percent water absorption of nylon 66 was reduced substantially on irradiation. Thermogravimetric analysis revealed that thermal stability of nylon 66 improved with increasing dose of radiation. Improvement of mechanical and thermal properties and reduction of water absorption of nylon 66 were due to the crosslinking of polyamide molecules made possible by the high energy radiation. Increase of crosslinking with increasing radiation dose was verified by the increase of gel content at higher doses. Differential scanning calorimetry showed that both melting and crystallization temperatures along with percent crystallinity of nylon 66 were decreased with the increasing dose of radiation leading to the development of more amorphous character in this semicrystalline polymer. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011.