Nuclear spin relaxation reveals a wealth of information concerning motional dynamics and morphology within a polymer system. The conventional breakdown of relaxation into discrete decay components is usually arbitrary and often ambiguous due to strong coupling and spin diffusion between domains. To avoid being limited by pre-determined models, we have explored the utility of maximum entropy regularization scheme to reconstruct the complete NMR spin relaxation distribution continuum. Case studies showed that the three characteristics of the distribution correlate with various aspects of polymer morphology and with physical properties. These positive results suggested that this approach has the potential of yielding profiles on polymer dynamics and information concerning phonon coupling between domains in complex polymer systems which are not previously accessible. Furthermore, the nondestructive nature of NMR gives this approach an extra advantage over conventional tests for ''in-situ'' studies of polymers.