Group interaction modeling (GIM) is used to predict the changes in the volume and, therefore, shrinkage of a wide variety of commonly encountered acrylate and methacrylate monomers during polymerization. The predictions of the model are in excellent agreement with experimental data available in the literature. It is demonstrated that, given appropriate estimations of the ultimate matrix morphology, GIM can be used to give estimates of polymerization shrinkage in three-dimensional crosslinked. polymer networks that relate well to experimental data available for dental composite matrices. GIM provides a very useful framework within which the phenomenon of polymerization shrinkage can be considered. The approach challenges certain common misconceptions relating conversion to shrinkage. The limitations of this approach are discussed, and targets for future research are clearly outlined that could extend the scope of this methodology to encompass novel systems for which morphological information is not available. (C) 2003 Wiley Periodicals, Inc.