To ascertain the potential impact of the restricted parametrization on accuracy, we compared the agreement of the bonded distributions of the fragments from our previous parameterization approach with those of the present work. Figure illustrates the angular distributions of a specific angle of the HS3 and HS30 fragments, respectively, for both approaches. In each diagram, the distribution of the optimized coarse-grained model is compared with the mapped reference. The complete set of distributions for these two fragments is given in the Supporting Information, Figure .