The rapid development of modern electrical equipment toward miniaturization and high power puts forward stringent requirements to the mechanical reliability, dielectric property, and heat resistance of electrical insulating materials. Simultaneous integration of all these properties for mica-based materials remains unresolved. Herein, inspired by the three-dimensional (3D) chitin nanofiber framework within the layered architecture of natural nacre, we report a large-area layered mica-based nanopaper containing a 3D aramid nanofiber framework, which is prepared by a sol−gel−film transformation process. The coupling of 3D aramid nanofiber framework and oriented mica nanoplatelets imparts the nanopaper with good mechanical strength, particularly outstanding ductility (close to 80%) and toughness (up to 109 MJ m −3 ), which are 4−240 and 6−220 times higher than those of all other nacre-mimetics. Meanwhile, the excellent mechanical properties are integrated with high dielectric strength (164 kV mm −1 ), excellent heat resistance (T g = 268 °C), good solvent resistance, and nonflammability, much better than conventional mica-based materials. Additionally, we successfully demonstrate its continuous production in the form of nanotape. The fabulous multiproperty combination and continuous production capability render the mica-based nanopaper a very promising electrical insulating material in miniaturized high-power electrical equipment.