Self‐Adhesive Polydimethylsiloxane Foam Materials Decorated with MXene/Cellulose Nanofiber Interconnected Network for Versatile Functionalities

Abstract Polydimethylsiloxanes (PDMS) foam as one of next‐generation polymer foam materials shows poor surface adhesion and limited functionality, which greatly restricts its potential applications. Fabrication of advanced PDMS foam materials with multiple functionalities remains a critical challenge. In this study, unprecedented self‐adhesive PDMS foam materials are reported with worm‐like rough structure and reactive groups for fabricating multifunctional PDMS foam nanocomposites decorated with MXene/cellulose nanofiber (MXene/CNF) interconnected network by a facile silicone foaming and dip‐coating strategy followed by silane surface modification. Interestingly, such self‐adhesive PDMS foam produces strong interfacial adhesion with the hybrid MXene/CNF nano‐coatings. Consequently, the optimized PDMS foam nanocomposites have excellent surface super‐hydrophobicity (water contact angle of ≈159 o ), tunable electrical conductivity (from 10 −8 to 10 S m −1 ), stable compressive cyclic reliability in both wide‐temperature range (from −20 to 200 o C) and complex environments (acid, sodium, and alkali conditions), outstanding flame resistance (LOI value of >27% and low smoke production rate), good thermal insulating performance and reliable strain sensing in various stress modes and complex environmental conditions. It provides a new route for the rational design and development of advanced PDMS foam nanocomposites with versatile multifunctionalities for various promising applications such as intelligent healthcare monitoring and fire‐safe thermal insulation.