Abstract:Compounds that can gelate aqueous solutions offer an intriguing toolbox to create functional hydrogel materials for biomedical applications. Here we show that amphiphilic Janus dendrimers with low molecular weights can readily form selfassembled fibers at very low mass proportion (0.2 per cent by mass) creating supramolecular hydrogels (G'>>G'') with outstanding mechanical properties, where the storage modulus G'>1000 Pa. The G' and gel melting temperature can be tuned by modulating the position or number of hydrophobic alkyl chains in the dendrimer structure, thus enabling an exquisite control over the mesoscale material properties in these molecular assemblies. The gels are formed within seconds by simple injection of ethanol-solvated dendrimers into an aqueous solution. Cryogenic transmission electron microcopy, small-angle x-ray scattering and scanning electron microscopy were used to confirm the fibrous structure morphology of the gels. Furthermore, we show that the gels can be efficiently loaded with different bioactive cargo, such as active enzymes, peptides or small molecule drugs to be used for sustained release in drug delivery.