Heating treatment is widely used in the preparation of metallic materials with controlled phase behavior and mechanical properties. However, for the soft materials assembled by short peptides, especially simple dipeptides, the detailed influences of heating treatment on the structures and functions of the materials remain largely unexplored. Here we showed that by thermal annealing or quenching of aromatic peptide solutions under kinetic control, we are able to control the self-assembly of peptide into materials with distinct phase behavior and macroscopic properties. The thermal annealing of the heated peptide solutions will lead to the formation of large nanobelts or bundles in solution, and no gels will be formed. However, by quenching the heated peptide solution, a self-supporting hydrogel will be formed quickly. Structure analysis revealed that the peptides preferred to self-assembled into much thinner and flexible nanohelices during quenching treatment. Moreover, the stability of the gels further increased with the repeated heating and quenching cycling of the peptide solutions. The results demonstrated that the heat treatment can be used to control the structure and function of self-assembled materials in a way similar to that of the conventional metallic or alloy materials. (C) 2020 Elsevier Inc. All rights reserved.