Bitumen derived from crude oil by fractional distillation has been used in the nuclear industry as a radioactive waste encapsulation matrix. When subjected to alpha, beta and gamma self-irradiation, this organic matrix undergoes radiolysis, generating hydrogen bubbles and modifying the physical and chemical properties of the material. In this paper, the effects of irradiation on bitumen materials, especially in terms of its physical, chemical, structural and rheological properties, were characterized at radiation doses ranging from 1 to 7 MGy. An increase in the shear viscosity and melt yield stress was observed with increasing doses. Similarly, the elastic and viscous moduli (G' and G '') increase with the dose, with a more pronounced increase for G' that reflects enhanced elasticity arising from radiation-induced cross-linking. In addition, a low-frequency plateau is observed for G', reflecting pseudo-solid behavior and leading to an increase of the complex viscosity. This behavior is due to increased interactions between asphaltene particles, and to aromatization of the bitumen by gamma-radiations. Cross-linking of bitumen enhances its strength, as confirmed by various techniques (modulated DSC, DTA/TGA, SEC, FTIR and XRD). (C) 2013 Published by Elsevier B.V.