Abstract Palladium-catalysed reductive alkylation of monosubstituted ureas has been studied in the presence of aldehydes and using molecular hydrogen as a clean reductant. Unsymmetrical N, N′-disubstituted ureas were formed in good to excellent isolated yields (60–93%) without the production of salt waste. This reaction was incorporated to a one-pot, solvent-free sequence involving the alkylation of monosubstituted ureas generated in situ ...