Pathway-Driven Peptide–Bioglass Nanocomposites as the Dynamic and Self-Healable Matrix

Peptide hydrogels have recently emerged as potential biomaterials for designing synthetic scaffolds in tissue engineering. We demonstrate pathway-controlled self-assembly of peptide amphiphile 1 to furnish kinetically controlled nanofibers (1NF) and thermodynamically stable twisted helical bundles (1TB). These supramolecular nanostructures with varied persistence lengths promote in situ mineralization to yield templated bioactive glass composites, 1NFBG and 1TBBG – resorbable, mesoporous, and degradable biomaterials as bone scaffolds. The structural features of the hydrogel composites are investigated extensively with microscopic characterization, energy-dispersive X-ray spectroscopy, Raman spectroscopy, and XPS to conclude 1TBBG as the superior material with higher percentage of open network structures as obtained from ratios of nonbridging and bridging oxygen. The hydrogel composites show excellent dynamic and self-healing behavior from rheological studies, especially the elastic modulus of 1TBBG being almost comparable to natural bone. Upon incubation in simulated body fluid, the bioglass composites illustrate tunable bioactive response mediated by the structural and topological control to induce the deposition of multiphasic calcium phosphate along with octacalcium phosphate and carbonate hydroxyapatite. Finally, such spatiotemporal composites facilitate stiffness-controlled osteoblast cellular interactions to support U2OS subsistence in the hydrogel matrix, highlighting their potential as a substrate for osteoblast growth for prolonged culture periods and in 3D bone tissue modeling.