We report on the development of bioinspired cardiac scaffolds made from electroconductive acid-modified silk fibroin-poly(pyrrole) (AMSF+PPy) substrates patterned with nanoscale ridges and grooves reminiscent of native myocardial extracellular matrix (ECM) topography to enhance the structural and functional properties of cultured human pluripotent stem cells (hPSC)-derived cardiomyocytes. Nanopattern fidelity was maintained throughout the fabrication and functionalization processes, and no loss in conductive behavior occurred due to the presence of the nanotopographical features. AMSF+PPy substrates were biocompatible and stable, maintaining high cell viability over a 21-day culture period while displaying no signs of PPy delamination. The presence of anisotropic topographical cues led to increased cellular organization and sarcomere development, and electroconductive cues promoted a significant improvement in the expression and polarization of connexin 43 (Cx43), a critical regulator of cell-cell electrical coupling. The combination of biomimetic topography and electroconductivity also increased the expression of genes that encode key proteins involved in regulating the contractile and electrophysiological function of mature human cardiac tissue.

Flexible and conductive biocompatible materials are attractive candidates for a wide range of biomedical applications including implantable electrodes, tissue engineering, and controlled drug delivery. Here, we demonstrate that chemical and electrochemical polymerization techniques can be combined to create highly versatile silk-conducting polymer (silk-CP) composites with enhanced conductivity and electrochemical stability. Interpenetrating silk-CP composites were first generated via in situ deposition of polypyrrole during chemical polymerization of pyrrole. These composites were sufficiently conductive to serve as working electrodes for electropolymerization, which allowed an additional layer of CP to be deposited on the surface. This sequential method was applied to both 2D films and 3D sponge-like silk scaffolds, producing conductive materials with biomimetic architectures. Overall, this two-step technique expanded the range of available polymers and dopants suitable for the synthesis of mechanically robust, biocompatible, and highly conductive silk-based materials.

Over the past few decades, Bombyx mori silk fibroin has become a ubiquitous material for applications ranging from biomedical devices to optics, electronics, and sensing, while also showing potential in the food supply chain and being re-engineered as a functional material for architecture and design-related applications. Its widespread use derives from its unique properties, including biocompatibility, edibility, optical transparency, stabilization of labile compounds, and the ability to controllably change conformation and degrade in a programmed way. This review discusses recent and pivotal silk-based devices in which the presence of silk brings added value in terms of functionality, as demonstrated in a broad variety of fields. First, it gives an overview of silk's natural structure and main properties in terms of cross-linking, biocompatibility, and biodegradability to provide the reader with the necessary toolbox to fully make use of silk's multifaceted properties. Then, multifunctional silk-based devices are discussed highlighting the advantage of using silk over more traditional materials. Representative devices from both established and emerging applications for silk are examined. Finally, a roadmap for the next generation of silk-based devices is laid out.