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Polyacrylonitrile (PAN) carbon fibers are often used to prepare high-performance paper-based materials owing to their high strength, good electrical and thermal conductivity, and superior comprehensive properties. In this study, a novel method for preparing PAN-based carbon fibers by centrifugal spinning was developed, and a stable and homogeneous PAN carbon fiber paper was successfully obtained. Subsequently, the formation process, microscopic morphology, electrical conductivity, electrochemical performance and hydrophobicity of the PAN carbon fiber paper were studied and evaluated. The results showed that the electrical conductivity of the PAN carbon fiber paper prepared via this method reached 43.250 s·cm−1, resistivity was as low as 0.023–0.033 Ω·cm, and contact angle exceeded 140°. This study adopted a new method to prepare PAN carbon fiber paper, which provided another method for the preparation of high-performance fiber paper.