Nature is enriched with a wide variety of complex, synergistic and highly functional protein-based multicomponent assemblies.

DBS is an efficient, versatile, low-molecular-weight gelator with a wide-range of industrial applications – greater understanding of its self-assembly and the creation of new derivatives are expanding the scope of this fascinating family of gels.

We report a novel gelator functionalised with hydrazides (as replacements for carboxylic acids) which, as a result, is able to assemble into hydrogels across a wide pH range – this gelator exhibits pH-switchable dye adsorption–desorption dependent on protonation of the target dyes and their resulting interactions with the self-assembled gel nanofibres.

Self-assembled nanofibers are ubiquitous in nature and serve as inspiration for the design of supramolecular hydrogels. A multicomponent approach offers the possibility of enhancing tunability and functionality of this class of materials. We report on the synergistic multicomponent self-assembly involving a peptide amphiphile (PA) and a 1,3:2,4-dibenzylidene-D-sorbitol (DBS) gelator to generate hydrogels with tunable nanoscale morphology, improved stiffness, enhanced self-healing, and stability to enzymatic degradation. Using induced circular dichroism of Thioflavin T (ThT), electron microscopy, small-angle neutron scattering (SANS), and molecular dynamics approaches we confirm that the PA undergoes self-sorting while the DBS-gelator acts as an additive modifier for the PA nanofibers. The supramolecular interactions between the PA and DBS gelators result in improved bulk properties and cytocompatibility of the two-component hydrogels as compared to the single component systems. The tunable mechanical properties, self-healing ability, resistance to proteolysis, and biocompatibility of the hydrogels suggest future opportunities for the hydrogels as scaffolds for tissue engineering and drug delivery vehicles.

Hybrid hydrogels combining both a low molecular weight gelator (LMWG, 1,3:2,4-dibenzylidene-D-sorbitol–p,p′-dicarboxylic acid) and a polymer gelator (PG, agarose) are reported. The dynamic assembly of the LMWG is explored in the absence and presence of the PG using NMR and CD methods. It is shown that the LMWG still assembles into chiral nanofibres in the presence of a nanoscale PG network, although the kinetics of assembly are somewhat modified. As such, these hybrid materials can be considered as self-sorting multi-gelator gels. Importantly, the LMWG retains its pH-responsive character and can be assembled and disassembled within the PG network, which acts to retain the overall integrity of the gel. As such, these materials demonstrate how the responsive nature of an LMWG can be combined with the greater resilience of a PG network to yield novel materials with hybrid performance.