To achieve desired physicochemical and biochemical activities of optically active molecules at targetted sites in biological systems, tuning of chiral sense by varying internal conditions (e.g., pH) is of utmost importance. However, it has been a challenge to gain the balance of non-covalent interactions required for chiral transformations merely by deviations in biochemical environment. Herein, pH-controlled chirality of supramolecular nanostructures obtained from coassembly of phenylalanine-derived gelator and achiral cationic polyacrylamide has successfully been achieved. Specifically, any changes in the pH remarkably influence the chirality of these nanostructures. For instance, coassembled hydrogels possessing l -enantiomer provide right-handed nanostructures at pH