Isocyanurate-oxazolidone polymers were synthesized by using various reactant stoichiometry of a diglycidyl ether of bisphenol-A (DGEBA) and a polymeric diphenyl methane diisocyanate (pMDI). The reaction was catalyzed by tris-2,4,6-dimethylaminoethylphenol (Ancamine K54). The effects of stoichiometry that the reaction had on the molecular structure and mechanical and thermomechanical properties were evaluated. Two main structures obtained from the reaction of DGEBA with pMDI, namely isocyanurate and oxazolidone, were clearly shown by Fourier transformed infrared spectroscopy (FTIR) analyses. It was found that the amount of DGEBA present determines the amount of oxazolidone formed. Where excess DGEBA was used, structural transformation reaction from isocyanurate to oxazolidone was observed. The amount of pMDI, on the other hand, influenced the amount of isocyanurate structure formed. As the relative amounts of isocyanurate and oxazolidone contents changed with stoichiometry of the reactants, the effects on the crosslink density in the samples were clearly shown by both mechanical and thermomechanical measurements.