The possibility of using differential pre-heating prior to supramolecularg elation to control the balance between hydrogen-bonding and aromatic stacking interactions in supramolecular gels and obtain consequents ystematic regulation of structure and properties is demonstrated. Using am odel aromatic peptide amphiphile, Fmoc-tyrosylleucine (Fmoc-YL) and ac ombination of fluorescence, infrared, circular dichroism and NMR spectroscopy,i ti ss hown that the balance of these interactions can be adjusted by temporary exposure to elevated temperatures in the range 313-365 K, followed by supramolecular locking in the gel state by cooling to room temperature. Distinct regimes can be identified regarding the balance between H-bonding and aromatic stacking interactions, with at ransition point at 333 K. Consequently,g els can be obtained with customizable properties,i ncluding supramolecular chirality and gel stiffness. The differential supramolecular structures also result in changes in proteolytic stability, highlighting the possibility of obtaining ar ange of supramoleculara rchitectures from as ingle molecular structure by simply controlling the pre-assemblyt emperature.[a] Dr.