N,N'-dialkylurea and an .alpha.,.beta.-unsaturated nitrile are reacted to form a cyclic N,N'-dialkylurea containing an imine group on a ring carbon. This compound is useful as an intermediate in the formation of N,N'-dialkylpropyleneureas by hydrogenation followed by hydrogenolysis to remove the imine group. Using N,N'-dimethylurea and acrylonitrile as the starting materials one can arrive at N,N'-dimethylpropyleneurea which is a compound useful as an organic solvent and known by its acronym, DMPU.