Molecular Insights Into the Assembly of PEDOT:PSS on Nanocellulose Surfaces

Conducting polymers (CPs) are widely recognized for their exceptional electronic, mechanical, and thermal properties, making them a preferable choice for flexible electronics, energy storage, and optoelectronic applications. The incorporation of biopolymers such as nanocellulose into CPs is an important strategy for future green technologies such as bioelectronics, energy storage and smart textiles. However, nanoscale organization of CPs and nanocellulose still needs to be addressed for their use in these devices. In this study, we performed atomistic molecular dynamics simulations to understand the interaction and organization of CP poly(3,4‐ethylene‐dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) on crystalline cellulose surface (CCS). First, we calculated the interaction of a single chain of PEDOT on various CCSs using the potential of mean force (PMF). We took two types of CCSs, namely, native CCS (CCS Native ) and TEMPO‐oxidized CCS (CCS TEMPO ) and studied the interaction of PEDOT with different planes of CCS, namely hydrophobic (100) and hydrophilic (010). Next, to gain understanding of the microscopic structure of PEDOT:PSS onto the CCS, we performed bulk molecular dynamic simulations of PEDOT:PSS on CCS. The simulations provide insights that uncover key structural features of PEDOT:PSS such as PEDOT chain organization, and interfacial interactions with the CCS. By bridging atomistic insights with microscopic properties, this work paves the way for designing next‐generation composites, combining the sustainable versatility of CCSs with the high‐performance characteristics of PEDOT:PSS, tailored for organic electronic devices.