A bisphenol A dicyanate resin, BADCy, was toughened by incorporating polysulfone, PSU, at various compositions. The catalyst system used was a mixture of copper acetylacetonate and nonylphenol, Phase separation and rheokinetics were studied through curing. The blends seemed to have a LCST behavior, and the presence of PSU did not affect the polycyclotrimerization kinetics. The phase structure, thermal, and mechanical properties of the final network were investigated as a function of the PSU content and cure temperature. The toughness of the BADCy/PSU blends was closely related to their final morphology, increasing with the amount of phase inversion. The mechanical properties were not affected by the addition of the thermoplastic.