Miniaturized, integrated, and functional electronic devices generate a large amount of heat accumulation during operation, which significantly affects the reliability, durability, and safety of electronic devices. In severe cases, it may even lead to fires. Therefore, the development of insulation composite materials with thermal conductivity and flame-retardant properties is particularly important. In this study, we propose an in-situ mineralization strategy to prepare insulation composite materials with thermal conductivity and flame-retardant properties. By dissolving and preparing a gel film, Al3+ and Zn2+ retained inside the lignocellulose are in situ mineralized to form Al(OH)3 and ZnO, and introducing inorganic blocks with high insulation performance (industrial waste mica tailings and synthetic mica). The prepared film has excellent tensile strength (117.4 MPa), low dielectric loss, high dielectric strength (83.8 kV mm−1), high insulation resistance, four times higher thermal conductivity than the unmineralized film, and excellent flame-retardant properties. Meanwhile, the environmental impact of the composite film is much lower than that of petrochemical-based plastic films and can easily degrade under natural conditions within 32 days. It is a composite material that meets the standards of the new electrical insulation field, and the in-situ mineralization strategy can also provide ideas for the preparation of high-performance lignocellulose-based materials.