A reliable and convenient protocol for MCRs between 2-aminopyrimidine, aldehydes and isonitriles is described. Toluene was chosen as the reaction solvent based on mechanistic reasoning. The product mixtures were found to contain a single imidazo[1,2-a]pyrimidine product in each case, which were isolated and purified by precipitation and crystallization. Chromatographic recovery from filtrates raised the total yields to 49-66%. The procedure provides a practical alternative to hitherto reported methods in which formation of multiple products was observed.