The prediction of thermal and mechanical properties of amine-cured epoxy resins by group interaction modelling is presented. The derivation of the group interaction based approach to the prediction of macroscopic engineering properties of both linear and crosslinked epoxy resins is described with specific application to MY721 resin. The glass transition temperature, bulk and tensile modulus and linear thermal expansion coefficient of tetraglycidyl 4,4′-diaminodiphenylmethane (TGDDM) cured with 4,4′-diaminodiphenyl sulphone (DDS) are estimated using the model and compared with results from dynamic mechanical experiments. The glass transition of TGDDM/DDS is calculated to occur at approximately 248 °C and the reasons for a secondary peak in the spectrum cured to 180 °C are given. The bulk and tensile modulus of TGDDM/DDS are calculated to be 7.54 GPa and 5.34 GPa, respectively.