Silks are natural fibrous protein polymers that are spun by silkworms and spiders. Among silk variants, there has been increasing interest devoted to the silkworm silk of B. mori, due to its availability in large quantities along with its unique material properties. Silk fibroin can be extracted from the cocoons of the B. mori silkworm and combined synergistically with other biomaterials to form biopolymer composites. With the development of recombinant DNA technology, silks can also be rationally designed and synthesized via genetic control. Silk proteins can be processed in aqueous environments into various material formats including films, sponges, electrospun mats and hydrogels. The versatility and sustainability of silk-based materials provides an impressive toolbox for tailoring materials to meet specific applications via eco-friendly approaches. Historically, silkworm silk has been used by the textile industry for thousands of years due to its excellent physical properties, such as lightweight, high mechanical strength, flexibility, and luster. Recently, due to these properties, along with its biocompatibility, biodegradability and non-immunogenicity, silkworm silk has become a candidate for biomedical utility. Further, the FDA has approved silk medical devices for sutures and as a support structure during reconstructive surgery. With increasing needs for implantable and degradable devices, silkworm silk has attracted interest for electronics, photonics for implantable yet degradable medical devices, along with a broader range of utility in different device applications. This Tutorial review summarizes and highlights recent advances in the use of silk-based materials in bio-nanotechnology, with a focus on the fabrication and functionalization methods for in vitro and in vivo applications in the field of tissue engineering, degradable devices and controlled release systems.

A nacre-like multilayer filtration membrane is developed by integration of computational simulation and experimental fabrication.

Significance: The majority of deformable actuators rely on synthetic materials with stimuli-responsive properties to execute the system, limiting their use in vivo. We designed and built a new class of bionic actuator entirely out of biocompatible and biodegradable materials. Stimuli-responsive genetically engineered silk–elastin-like proteins (SELPs) and cellulose nanofibers (CNFs) are combined to fabricate an actuator system that could effectively respond to physical and chemical stimuli. Programmable and reversible deformations in response to the stimuli have been achieved with this actuator. The SELP/CNF actuator provides an option for fields such as in vivo biomedical soft robotics and biomimetic devices where biocompatibility, biodegradability, biomedical signals recognition, and durability are desired.

Silk and elastin are exemplary protein materials that exhibit exceptional material properties. Silk is uniquely strong, surpassing engineering materials such as Kevlar and steel, while elastin has exquisite flexibility and can reversibly fold into a more structured form at high temperatures when many other proteins would unfold and denature. This phenomenon in elastin is termed the inverse temperature transition. It is a reversible, controllable process that motivates applications in drug delivery, shape change materials, and biomimetic devices. Silk-elastinlike protein polymers (SELPs), which combine repeating B. mori silk and elastin blocks, have been introduced as biologically inspired materials that combine the distinctive properties of the component parts to achieve strong and extensible, tunable biomaterials. Here, we considered a single SELP sequence to examine temperature transition effects at the molecular scale. SELP molecular models were created using Replica Exchange Molecular Dynamics, an accelerated sampling method, and confirmed in experiment by comparing secondary structure distributions. A molecular collapse of the SELP molecule was observed with increased temperature in both molecular simulation and experiment. Temperature-specific differences were observed in the mechanical properties and the unfolding pathways of the polypeptide. Using the Bell–Evans model, we analyzed the free energy landscape associated with molecular unfolding at temperatures below and above the transition temperature range (T_t) of the polypeptide. We found that at physiological pulling rates, the energy barrier to unfold SELPs was counterintuitively higher above T_t. Our findings offer a foundational perspective on the molecular scale mechanisms of temperature-induced phase transition in SELPs, and suggest a novel approach to combine simulation and experiment to study materials for multifunctional biomimetic applications.

Adaptive hydrogels tailor-made from silk-elastin-like proteins (SELPs) possess excellent biocompatibility and biodegradability with properties that are tunable and responsive to multiple simultaneous external stimuli. To unravel the molecular mechanisms of their physical response to external stimuli in tandem with experiments, here we predict and measure the variation in structural properties as a function of temperature through coarse-grained (CG) modeling of individual and crosslinked SE_8Y and S₄E_8Y molecules, which have ratios of 1 : 8 and 4 : 8 of silk to elastin blocks respectively. Extensive structural reshuffling in single SE_8Y molecules led to the increased compactness of the structure, whereas S₄E_8Y molecules did not experience any significant changes as they already adopted very compact structures at low temperatures. Crosslinking of SE_8Y molecules at high concentrations impeded their structural transition at high temperatures that drastically reduced the degree of deswelling through extensive suppression of the structural shuffling and the trapping of the molecules in high potential energy states due to inter-molecular constraints. This integrative experimental and computational understanding of the thermal response in single molecules of SELPs and their crosslinked networks should lead to further improvements in the properties of SELP hydrogels through predictive designs and their wider applications in biomaterials and tissue engineering.