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Hydrogels are widespread soft materials, which can serve a wide range ofapplications. The control over the viscoelastic properties of the gel is ofparamount importance. Ongoing environmental issues have raised the consumer'sconcern towards the use of more sustainable materials, including hydrogels.However, are greener materials compatible with high functionality? In asafe-by-design approach, this work demonstrates that functional hydrogels within situ responsivity of their elastic properties by external stimuli can bedeveloped from entirely ``sustainable'' components, a biobased amphiphile andbiopolymers (gelatin, chitosan and alginate). The bioamphiphile is astimuli-responsive glycolipid obtained by microbial fermentation, which canself-assemble into fibers, but also micelles or vesicles, in water under highdilution and by a rapid variation of the stimuli. The elastic properties of thebioamphiphile/biopolymer interpenetrated hydrogels can be modulated byselectively triggering the phase transition of the glycolipid and/or thebiopolymer inside the gel by mean of temperature or pH.

In situ stimulation of self-assembly tunes the elastic properties of interpenetrated glycolipid-biopolymer biobased hydrogels