SynopsisN-phenylated aromatic polyureas were synthesized by the polyaddition of dianilino compounds to aromatic diisocyanates in sym-tetrachloroethane at around 100°C. Factors that influence the reaction, such as monomer concentration, reaction solvent, catalyst, temperature, and time, were studied to optimize the conditions for the preparation of high molecular weight polymers. Compared with the analogous unsubstituted aromatic polyureas, the N-phenylated polyureas were almost amorphous and soluble in a variety of solvents and had low glass transition temperatures. Some of the polymers could be cast into transparent flexible films from chloroform solutions.