LAUSR

Cellulose nanofiber (CNF) is an advanced bio‐nanomaterial. However, the hydroxyl groups on the surface of CNFs are highly polar, leading to its weak interfacial compatibility with natural rubber (NR). Therefore, it is necessary to organically modify CNFs by silanization to improve the interfacial compatibility between CNFs and NR, which can then be used to prepare high‐performance CNF/NR composites. In this study, the effect of plasma‐activated pre‐silanization of CNFs on the vulcanization characteristics, mechanical properties, Payne effect, and dynamic mechanical properties of CNF/NR composites is investigated. The high‐energy impact of the plasma weakens the agglomeration of CNFs and increased the fiber surface roughness, providing a larger contact reaction area for the silanization reaction between the silane coupling agent and CNFs. The results show that the prepared CNF/NR composites have excellent physical and mechanical properties and processing safety. Compared with the unmodified CNF, its DIN wear increases by 4%, tensile strength increases by 23%, reinforcement factor increases by 7%, rolling resistance decreases by 6.3%, and Mooney viscosity decreases by 17.6%. Overall, this study presents a novel approach for the high‐value utilization of CNFs and the preparation of NR composites with exceptional properties, thereby establishing a solid foundation for the application of all‐steel treads.