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The dipeptide amphiphile Fmoc-Leu-Gly-OH has been induced to self-assemble into thin surface-supported hydrogel gel films and gap-spanning hydrogel membranes. The thickness can be closely controlled, giving films/membranes from tens of nanometers to millimeters thick. SEM and TEM have confirmed that the dipeptides self-assemble to form fibers, with the membranes resembling a dense "mat" of entangled fibers. The films and membranes were stable once formed. The films could be reversibly dried and collapsed, then reswollen to regain the gel structure.