Abstract: Novel self-assembling pentapeptides and peptides containing such self-assembling pentapeptides, self-assembled hydrogels, and methods of making and using the same are described. These pentapeptides, and peptides containing such pentapeptides, self-assemble under physiological conditions (e.g., in a physiological buffer under biologically acceptable conditions (e.g., pH?6-11)) into long fibrils with sequence-dependent fibrillary morphologies. The hydrogels comprise one or more these pentapeptides which make up the 3-dimensional nanofibrous network of the hydrogel structure. The hydrogels are shear-thinning hydrogels that have high storage moduli and high rates of recovery after destruction.