Two dimensional self-assembly of bis-acylureas having various functional end groups

► Bis-acylureas with various end functional groups were synthesized. ► They self-organize upon cooling from hot solutions forming superstructures. ► Unless the functionalities are bulky, rigid, or reactive, the bis-acylureas self-assemble with lamellar molecular packing. ► The resulting nanosheet structures have flat surfaces that are molecularly flat over hundreds of nanometers.