Many promising strategies have been developed for controlling the release of drugs from scaffolds, yet there are still challenges that need to be addressed in order for these scaffolds to serve as successful treatments. The RADA4 self-assembling peptide spontaneously forms nanofibers, creating a scaffold-like tissue-bridging structure that provides a three-dimensional environment for the migration of living cells. We have found that RADA4: (1) facilitates the regeneration of axons in the brain of young and adult hamsters, leading to functional return of behavior and (2) demonstrates robust migration of host cells and growth of blood vessels and axons, leading to the repair of injured spinal cords in rats.