Magneto- and photo-responsive hydrogels from the co-assembly of peptides, cyclodextrins, and superparamagnetic nanoparticles.

Dual response to external non-invasive stimuli, such as light and magnetic field, is a highly desirable property in soft nanomaterials with potential applications in soft robotics, tissue engineering, and life-like materials. Within this class of materials, hydrogels obtained from the self-assembly of low molecular weight gelators (LMWGs) are of special interest due to their ease of preparation and modification. Herein, we report a modular co-assembly strategy for a magneto- and photo-responsive supramolecular hydrogel based on the arylazopyrazole (AAP) modified pentapeptide gelator Nap-GFFYS, and β-cyclodextrin vesicles (CDVs) with superparamagnetic cobalt ferrite nanoparticles embedded in their membranes. Upon application of a magnetic field, a reversible increase in the storage modulus is observed during rheological measurements. Additionally, a gel rod could be manipulated with a weak permanent magnet, resulting in macroscopic bending of the rod. Furthermore, through irradiation with UV and visible light, respectively, the host-guest interaction between the AAP moiety and the hydrophobic cavity of the β-CD can be deactivated on demand, thus lowering the stiffness of the hydrogel reversibly.