Jianbin Sun, Man Liu, Shi Feng, Tianqi Jiang, Chengyao Liang, Jialiang Zhou, Yanhong Wei, Li Song, Yan Yu, Zexu Hu, Liping Zhu, Hengxue Xiang, Meifang Zhu
The increasing thermal and electrical demands of next-generation transformers and precision electronics necessitate the development of insulating materials that simultaneously exhibit high thermal conductivity, superior dielectric properties, and long-term reliability. Traditional aramid-based papers, while offering outstanding thermal stability and insulation, suffer from intrinsically low through-plane thermal conductivity. In this work, we report a nacre-inspired composite paper consisting of aramid nanofibers, guar gum, and mica (ANFs/GG/Mica), fabricated via a one-pot aqueous co-assembly process amenable to continuous manufacturing. Multivalent hydrogen bonding between amide groups, hydroxyl segments, and silanol surfaces forms a robust organic–inorganic interface, significantly reducing both interfacial thermal resistance and charge-carrier mobility. The optimized composite exhibits a through-plane thermal conductivity of 2.87 W m −1 K −1 at 150 °C and a dielectric breakdown strength of 86.9 MV m −1 , corresponding to enhancements of 62% and 28%, respectively, compared with pristine ANF paper. Notably, the composite paper retains over 70% of its mechanical strength after 168 h of ultraviolet (UV) aging, demonstrating excellent environmental stability. This work presents a flexible assembly strategy that leverages layered alignment and dense interfacial bonding to achieve a well-balanced combination of heat conduction, electrical insulation, and reliability. • One-pot assembly of nacre-inspired ANF/GG/Mica composite paper. • Guar-gum molecular bridges facilitate dense organic–inorganic interface. • Achieve a well-balanced of heat conduction, insulation, and reliability.