Rolling resistance is a key tire property considered in the design and manufacturing of tires. Usually rolling resistance is measured by an expensive quantitative tire test using a prototype final product, In order to speed up the development, efforts have been made to predict rolling resistance using samples rather than prototype tires. One such attempt is to correlate the mechanical loss factor tan(delta) to rolling resistance. However, this method is quite empirical and not useful if the influence of factors like polymer structure or filler on the rolling resistance is of interest. Especially for silica filled compounds or hybrid systems the correlation of rolling resistance with the loss factor is not successful. Combining dynamic mechanical measurements with the mastercurve technique and the separation and modeling of molecular relaxation processes yields an improved technique for predicting the rolling resistance.