Supramolecular Nanofibrous Peptide/Polymer Hydrogels for the Multiplexing of Bioactive Signals

The ability to provide multiple functions within a single scaffold biomaterial is a major goal in tissue engineering. Self-assembling peptide-based hydrogels are gaining significant attention as three-dimensional biomaterials because they provide a network of nanofibers similar to the native extracellular matrix while allowing the presentation of multiple biochemical cues for cell signaling. Herein, we combine a positively charged peptide amphiphile (PA) and the negatively charged synthetic polymer poly(sodium 4-styrenesulfonate) (PSS) to fabricate hybrid hydrogels through supramolecular self-assembly. PSS/PA hydrogels show rather high mechanical stiffness while being stable in buffered environment. The sulfonate functionality in PSS promotes hydrogel mineralization which can be controlled if undertaken in standard osteogenic medium. Loading proteins with different charges in the hydrogels reveals their ability to retain and sustain their release and indicates their potential for the controlled delivery of growth factors. Human mesenchymal stem cells encapsulated in PSS/PA hydrogels remain viable. The biomimetic nanofibrous structure of the hydrogels, together with multiplexing of bioactive signals, can provide a suitable environment for stem cell differentiation.