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Kevlar pulp treated with low-temperature plasma and nano cellulose fibrils (NCFs) have been introduced as reinforcements in the preparation for composite insulating paper with low relative permittivity, dielectric loss, good mechanical properties, and thermal stability. More polar groups of Kevlar fibers could be exposed after plasma treatment. Results showed that the relative permittivity of the composite paper containing 20% Kevlar pulp, 10% NCF, and 70% softwood pulp is decreased by 29.6% and the dielectric loss is decreased by 43.2% at 50 Hz, 25°, compared with the conventional paper formed by pure softwood pulp. The change was due to the introduction of Kevlar pulp with intrinsic low dielectric constant and loss, which decreases the whole polarizability of the paper. The mechanical properties of the composite paper became worse after introducing 20% Kevlar pulp. About 10% NCF can work as a mechanical reinforcement to compensate for the tensile and Yang's modulus loss. Scanning electron microscopy results showed that NCF could fill the void defects and improve the interface bonding of the fibers to enhance the paper mechanical properties. The composite paper also had better insulating and thermal properties than the conventional paper. It has been concluded that the Kevlar pulp/NCF/softwood pulp composite paper has the potential to replace the pure softwood paper for the application of high-voltage ac transformer insulation.