A huge and sustained growth number of urban vehicles incur concomitant problems, including enormous fuel consumption, CO2 emission and the progressively emerging haze. The development of low rolling resistance green tire plays a significant role in both fuel saving and air pollution issues. The overdependence of polymer materials on petrochemical resources can be alleviated by biomass development. Here, we brought out the strategy to fabricate elastomer from biobased chemicals—itaconic acid, mono alcohols and conjugated dienes aiming at sustainable resources and reducing CO2 emission. Combining the molecular structure design and silica-silane technology to tune the viscoelastic behavior of elastomer composites, we successfully manufactured silica/poly(di-n-butyl itaconate-co-butadiene) tire which achieved “B” level in rolling resistance of EU Tyre Label. The research opens an important way for reducing the dependence on petrochemical resources, saving fuel and cutting annual CO2 emission in elastomer field.