The influence of aliphatic chain lengths on supramolecular hydrogelation of naphthalene diimide-capped dipeptides is described. The dependence of the gelation pH as a function of chain lengths reveals an inverse linear relationship and the gelation pH values cover a broad range from pH 2 to pH 9. In addition, the presence of a n-octyl tail in the hydrogelator could enhance the ability of self-assembly in dilute solution.