This research is aimed to understand the growth mechanisms for self-assembly of dialkylated melamine derivatives. The dialkylated melamine derivatives with different alkyl chains (Mela-m-n) are able to self assemble with hydrochloric acid in dichloromethane to form 2D organic assemblies, exhibiting similar lamellar structures as Mela-n center dot HCl with identical alkyl chains. The most interesting finding is that the growth mechanism of Mela-n center dot HCl with identical alkyl chains is revealed to be layer growth, while Mela-m-n center dot HCl with asymmetric alkyl chains adopts a spiral growth mechanism The asymmetric alkyl chains in Mela-m-n may lead to the formation of dislocation, which is responsible for the spiral growth mechanism.