Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)
(PEDOT:PSS)-based
hydrogels have emerged as ideal interfacing materials for bioelectronics
because of their intriguing electrical, mechanical, and biological
properties. However, the development of high-performance PEDOT:PSS-based
hydrogels simultaneously achieving high conductivity, robust mechanical
properties, and accessibility for advanced manufacturing technologies
remains a critical challenge for further advancing such materials
toward practical applications. Herein, we develop a highly conductive,
intrinsically soft, tough yet stretchable PEDOT:PSS-based hydrogel
via a simple PSS-chain engineering strategy of introducing thermally
cross-linkable N-(hydroxymethyl)acrylamide segments.
The resultant PEDOT:PSS hydrogel exhibits high electrical conductivity
(1850 S m–1), high stretchability (>50%), low
Young’s
modulus (4 MPa), and superior toughness (400 kJ m–3), satisfying multiple property requirements for practical bioelectronic
applications. Based on this material, we further develop a novel PEDOT:PSS
ink with superior 3D printability for direct ink writing 3D printing,
enabling us to facilely fabricate bioelectronic devices like soft
skin electrodes comparable to commercial products via multi-material
3D printing.