Mechanically Adaptive Mixed Ionic-Electronic Conductors Based on a Polar Polythiophene Reinforced with Cellulose Nanofibrils

[Image: see text] Conjugated polymers with oligoether side chains are promising mixed ionic-electronic conductors, but they tend to feature a low glass transition temperature and hence a low elastic modulus, which prevents their use if mechanical robust materials are required. Carboxymethylated cellulose nanofibrils (CNF) are found to be a suitable reinforcing agent for a soft polythiophene with tetraethylene glycol side chains. Dry nanocomposites feature a Young’s modulus of more than 400 MPa, which reversibly decreases to 10 MPa or less upon passive swelling through water uptake. The presence of CNF results in a slight decrease in electronic mobility but enhances the ionic mobility and volumetric capacitance, with the latter increasing from 164 to 197 F cm(–3) upon the addition of 20 vol % CNF. Overall, organic electrochemical transistors (OECTs) feature a higher switching speed and a transconductance that is independent of the CNF content up to at least 20 vol % CNF. Hence, CNF-reinforced conjugated polymers with oligoether side chains facilitate the design of mechanically adaptive mixed ionic-electronic conductors for wearable electronics and bioelectronics.