Hydrogels have emerged as a promising bioelectronic interfacing material. This review discusses the fundamentals and recent advances in hydrogel bioelectronics.

Hydrogels of conducting polymers, particularly poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), provide a promising electrical interface with biological tissues for sensing and stimulation, owing to their favorable electrical and mechanical properties. While existing methods mostly blend PEDOT:PSS with other compositions such as non-conductive polymers, the blending can compromise resultant hydrogels’ mechanical and/or electrical properties. Here, we show that designing interconnected networks of PEDOT:PSS nanofibrils via a simple method can yield high-performance pure PEDOT:PSS hydrogels. The method involves mixing volatile additive dimethyl sulfoxide (DMSO) into aqueous PEDOT:PSS solutions followed by controlled dry-annealing and rehydration. The resultant hydrogels exhibit a set of properties highly desirable for bioelectronic applications, including high electrical conductivity (~20 S cm −1 in PBS, ~40 S cm −1 in deionized water), high stretchability (> 35% strain), low Young’s modulus (~2 MPa), superior mechanical, electrical and electrochemical stability, and tunable isotropic/anisotropic swelling in wet physiological environments.

Conducting polymers are promising material candidates in diverse applications including energy storage, flexible electronics, and bioelectronics. However, the fabrication of conducting polymers has mostly relied on conventional approaches such as ink-jet printing, screen printing, and electron-beam lithography, whose limitations have hampered rapid innovations and broad applications of conducting polymers. Here we introduce a highperformance 3D printable conducting polymer ink based on poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) for 3D printing of conducting polymers. The resultant superior printability enables facile fabrication of conducting polymers into high resolution and high aspect ratio microstructures, which can be integrated with other materials such as insulating elastomers via multi-material 3D printing. The 3D-printed conducting polymers can also be converted into highly conductive and soft hydrogel microstructures. We further demonstrate fast and streamlined fabrications of various conducting polymer devices, such as a soft neural probe capable of in vivo single-unit recording.