A correlation has been established between the dynamic storage modulus (E') and the mean cross polarization time constants 〈TCH〉 for a set of five morphologically diverse polymers, including one at two temperatures and one at two plasticizer concentrations. The correlation is only possible when the TCH values for all of the motional environments within the polymers are considered. An inversion recovery cross polarization (IRCP) NMR technique is used to obtain motional and morphological information from the main chain carbons of each polymer. After comparing simplified correlation functions for the two parameters, an experimental relationship between them is established that suggests that TCH and E' are both modulated by a similar distribution of molecular motions.