It is common to use crumb rubber as modifier in bitumen. Good performance of crumb rubber in bitumen has been reported in terms of improving characteristics like higher skid resistance, reducing noise, higher rutting resistance and longevity. However, due to the vulcanization, the polymeric crosslinked structure of crumb rubber suffers from inadequate dispersion and incompatibility in bitumen where storage stability becomes an issue. To solve this problem, partial surface devulcanization of the rubber via chemical and microbial surface activation was examined in this study showing both method can be effective to enhance rubber-bitumen interactions and subsequently storage stability of the rubberized bitumen. To ensure proper surface activation, it is important to thoroughly understand chemo-mechanics of bitumen containing rubber particles as well as underlying interaction mechanism at the molecular level. Therefore, this study integrates a multi-scale approach using density functional theory based computational modeling and laboratory experiments to provide an in-depth understanding of the mechanisms of interaction between surface activated rubber and bitumen. To do so, efficacy of various bio-modifiers was examined and compared it terms of both surface activation capability and durability of resulting rubberized bitumen. It was found that biomodifiers with various compositions can have either synergistic or antagonistic effect onchemo-mechanics of rubberized bitumen. The study was further extended to study the interplay of Polyphosphoric Acid (PPA) and these biomodified rubberized bitumens showing not all modifiers have high synergy with PPA in bitumens. Finally, durability of rubberized bitumen was studied in terms of its resistance to Ultraviolet (UV) aging. It was shown that there is a strong relation between composition of biomodified rubberized bitumen and its resistance to UV-aging.