Perylene dianhydride (PDA) hydrogels are made from highly accessible perylene diamic acid salts (PDAA salts) by a versatile protonation–hydrolysis mechanism. Very weak gels are formed initially by π-stacking of PDAAs and subsequent hydrolysis yields much stronger PDA hydrogels. Hydrogels are readily made at concentrations down to 0.5 mM, exhibit storage moduli around 600 Pa @ 1 mM and undergo significant syneresis in time.