Highly‐Strong and Highly‐Tough Alginate Fibers with Photo‐Modulating Mechanical Properties

Abstract The good combination of high strength and high toughness is a long‐standing challenge in the design of robust biomaterials. Meanwhile, robust biomaterials hardly perform fast and significant mechanical property changes under the trigger of light at room temperature. These limit the application of biomaterials in some specific areas. Here, photoresponsive alginate fibers are fabricated by using the designed azobenzene‐containing surfactant as flexible contact point for cross‐linking polysaccharide chains of alginate, which gain high mechanics through reinforced plastic strain and photo‐modulating mechanics through isomerization of azobenzene. By transferring molecular motion into macro‐scale mechanical property changes, such alginate fibers achieve reversible photo‐modulations on the mechanics. Their breaking strength and toughness can be photo‐modulated from 732 MPa and 112 MJ m⁻³ to 299 MPa and 27 MJ m⁻³, respectively, leading to record high mechanical changes among the developed smart biomaterials. With merits of good tolerance to pH and temperature, fast response to light, and good biocompatibility, the reported fibers will be suitable for working in various application scenarios as new smart biomaterials. This study provides a new design strategy for gaining highly‐strong and highly‐tough photoresponsive biomaterials.