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To more fundamentally understand the materials design of bitumen, we used the molecular scale calculation to predict properties and prepare asphalt materials. This review provides a conclusion on the material design, asphaltene models, bitumen models, and the applications of molecular simulation. The objectives of the investigation were the following: asphaltene models and bitumen models; thermo-mechanical properties calculation of bitumen; interfacial behavior; self-healing properties calculation of bitumen and aging and antiaging mechanisms of graphene modified bitumen.