Modern electrical devices are increasingly miniaturized and high-powered, leading to greater demands for advanced electrical insulating materials. Herein, multifunctional aramid nanofiber (ANF) insulating materials were prepared by in situ generation of hydroxyapatite (HAP) nanowires with a controllable aspect ratio. The dense network structure of ANF/HAP as well as the interlayer interactions resulted in the preparation of composite film materials with high tensile strength (102.35 MPa) and excellent electrical insulating properties (89.57 kV/mm). In particular, the fire-resistant and flame-retardant properties of the multilayer hot-pressed composite HAP/ANF paper were also greatly improved due to the properties of HAP. In addition, this study also provides a theoretical reference for the application of HAP flame retardants and provides ideas for the design of nanodielectric insulating materials.