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ABSTRACT Sustainable alternatives to petroleum‐based plastics are needed urgently, but biodegradable materials from renewable sources often suffer from inadequate mechanical properties. Here, we demonstrate a bio‐inspired strategy to enhance soy protein isolate (SPI) nanocomposites through surface modification of cellulose nanocrystal (CNC) reinforcing filler particles with a polydopamine (polyDOPA) coating via dopamine polymerization under alkaline conditions. This modification creates multifunctional interfaces at filler surfaces that enhance nanocomposite mechanical properties likely by simultaneously altering filler dispersion and filler–matrix interactions. PolyDOPA‐modified CNCs increase the tensile strength and elastic modulus of SPI films (plasticized with 50% glycerol) by more than threefold compared to unreinforced controls. Transmission electron microscopy, spectroscopic techniques, and thermal analysis reveal that polyDOPA coatings influenced nanocomposite structure across multiple length scales, tripling the effective diameter of the CNC inclusions, reducing the tendency of CNC nanocrystals to aggregate, and increasing the glass transition temperature. The increase in glass transition temperature suggests reduced SPI molecular mobility, which, along with micromechanical modeling, indicates the potential for improved interfacial interactions. Results reveal how polyDOPA‐modified CNCs influence the interphase behavior and filler dispersion of SPI‐glycerol nanocomposites, providing a pathway to further improve their performance for various applications, including packaging, membranes, and coatings. 

Abstract Spider dragline silk is known for its exceptional strength and toughness; hence understanding the link between its primary sequence and mechanics is crucial. Here, we establish a deep-learning framework to clarify this link in dragline silk. The method utilizes sequence and mechanical property data of dragline spider silk as well as enriching descriptors such as residue-level mobility (B-factor) predictions. Our sequence representation captures the relative position, repetitiveness, as well as descriptors of amino acids that serve to physically enrich the model. We obtain high Pearson correlation coefficients (0.76–0.88) for strength, toughness, and other properties, which show that our B-factor based representation outperforms pure sequence-based models or models that use other descriptors. We prove the utility of our framework by identifying influential motifs and demonstrating how the B-factor serves to pinpoint potential mutations that improve strength and toughness, thereby establishing a validated, predictive, and interpretable sequence model for designing tailored biomaterials. 

Abstract Microbially-synthesized protein-based materials are attractive replacements for petroleum-derived synthetic polymers. However, the high molecular weight, high repetitiveness, and highly-biased amino acid composition of high-performance protein-based materials have restricted their production and widespread use. Here we present a general strategy for enhancing both strength and toughness of low-molecular-weight protein-based materials by fusing intrinsically-disordered mussel foot protein fragments to their termini, thereby promoting end-to-end protein-protein interactions. We demonstrate that fibers of a ~60 kDa bi-terminally fused amyloid-silk protein exhibit ultimate tensile strength up to 481 ± 31 MPa and toughness of 179 ± 39 MJ*m⁻³, while achieving a high titer of 8.0 ± 0.70 g/L by bioreactor production. We show that bi-terminal fusion of Mfp5 fragments significantly enhances the alignment of β-nanocrystals, and intermolecular interactions are promoted by cation-π and π-π interactions between terminal fragments. Our approach highlights the advantage of self-interacting intrinsically-disordered proteins in enhancing material mechanical properties and can be applied to a wide range of protein-based materials. 

Mechanical stretch can activate long-lived changes in fibroblasts, increasing their contractility and initiating phenotypic transformations. This activation, critical to wound healing and procedures such as skin grafting, increases with mechanical stimulus for cells cultured in two-dimensional but is highly variable in cells in three-dimensional (3D) tissue. Here, we show that static mechanical stretch of cells in 3D tissues can either increase or decrease fibroblast activation depending upon recursive cell–extracellular matrix (ECM) feedback and demonstrate control of this activation through integrated in vitro and mathematical models. ECM viscoelasticity, signaling dynamics, and cell mechanics combine to yield a predictable, but nonmonotonic, relationship between mechanical stretch and long-term cell activation. Results demonstrate that feedback between cells and ECM determine how cells retain memory of mechanical stretch and have direct implications for improving outcomes in skin grafting procedures. 

A major challenge in synthesizing strong and tough protein fibers based on spider silk motifs is understanding the coupling between protein sequence and the postspin drawing process. We clarify how drawing-induced elongational force affects ordering, chain extension, interchain contacts, and molecular mobility through mesoscale simulations of silk-based fibers. We show that these emergent features can be used to predict mechanical property enhancements arising from postspin drawing. Simulations recapitulate a purely process-dependent mechanical property envelope in which order enhances fiber strength while preserving toughness. The relationship between chain extension and crystalline domain alignment observed in simulations is validated by Raman spectroscopy of wet-spun fibers. Property enhancements attributed to the progression of anisotropic extension are verified by mechanical tests of drawn silk fibers and justified by theory. These findings elucidate how drawing enhances properties of protein-based fibers and shed light on how to incorporate this effect into predictive models. 

Surgical reattachment of tendon to bone is a clinical challenge, with unacceptably high retear rates in the early period after repair. A primary reason for these repeated tears is that the multiscale toughening mechanisms found at the healthy tendon enthesis are not regenerated during tendon -to -bone healing. The need for technologies to improve these outcomes is pressing, and the tissue engineering community has responded with many advances that hold promise for eventually regenerating the multiscale tissue interface that transfers loads between the two dissimilar materials, tendon, and bone. This review provides an assessment of the state of these approaches, with the aim of identifying a critical agenda for future progress. 

Blending diverse amyloid-silk proteins enables creation of mechanically programmable composite fibers and adjusting the blending ratio provides precise control over fiber mechanical behavior to specifically tailor them for diverse applications.