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[Display omitted] • A flexible nanocomposite paper is prepared based on ultralong hydroxyapatite nanowires and aramid nanofibers. • The networked framework, layered structure and interfacial interactions enhance mechanical properties of the paper. • The flexible nanocomposite paper exhibits high dielectric breakdown strength, thermal stability, and flame retardancy. With the increasing popularity of modern electronic devices in the fifth-generation (5G) era, high-performance and high-safety electrically insulating materials with good mechanical flexibility and strength, high thermal stability and fire resistance are urgently needed. Herein, we report a highly flexible, thermally stable, and fire-retardant nanocomposite paper with high dielectric breakdown strength and mechanical strength by synergistically integrating one-dimensional ultralong hydroxyapatite (HAP) nanowires and aramid nanofibers (ANFs) through the vacuum-assisted filtration process. The as-prepared HAP/ANF nanocomposite paper has a nanowire/nanofiber networked framework and a layered structure, and exhibits high tensile strength (73.5 MPa), fracture strain (7.4 %), folding durability (1396 times under a loading weight of 9.8 N), excellent flexibility, and good processibility. Notably, the HAP/ANF nanocomposite paper has a superior dielectric breakdown strength (92.4 kV mm−1), high thermal stability and flame retardancy in comparison with the commercial Nomex T410 electrical insulation paper. The multifunctional HAP/ANF nanocomposite paper is promising for applications in miniaturized and flexible electronic devices, high-voltage electrical insulation equipments, and fire-retardant and high-temperature fields. [ABSTRACT FROM AUTHOR]