Description:
<jats:title>Abstract</jats:title><jats:p>Organohydrogels (OHGs) are soft materials with antagonistic hydrophilic and hydrophobic domains that have great interest for many different applications. This study presents the preparation of mechanically strong OHGs with shape‐memory function by incorporating semicrystalline organo‐microgels within the pores of silk fibroin (SF) scaffolds. In the first step, SF cryogels with various pore diameters between 26 ± 8 and 17 ± 4 µm are synthesized by cryogelation of aqueous SF solutions at concentrations between 5 and 20 w/v%. In the second step, the pores of SF scaffolds are filled with an organogel precursor solution containing n‐octadecyl acrylate (C18A), acrylic acid, <jats:italic>N</jats:italic>,<jats:italic>N</jats:italic>'‐methylene(bis)acrylamide, and an initiator. Once the free‐radical polymerization took place inside the pores, OHGs containing organo‐microgels of various sizes are obtained. The incorporation of the organogel component in the cryogels generates crystalline areas due to the side‐by‐side packed C18 side chains. OHGs' melting temperature and crystallinity level can be varied from 42 to 54 °C and from 2 to 16%, respectively. The stiffness of OHGs increases from 5.9 ± 0.5 to 18 ± 1 MPa with increasing SF concentration from 5 to 20 w/v%, which is attributed to the decreasing pore size of the cryogels and increasing thickness of the pore walls.</jats:p>