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The weak interfacial adhesion between carbon fiber (CF) and polyetheretherketone (PEEK) is a longstanding problem that hinders the applications of CF/PEEK composites. To solve this problem, a mixture sizing agent containing hydroxylated boron nitride (BNO) and polyetherimide (PEI) is synthesized to coat CF. In this study, BNO is synthesized via the liquid exfoliation method. The interfacial adhesion between CF and PEEK is improved using a mixture sizing layer of BNO and PEI on CF. The synergistic effects of hydrogen bonding, π-π interaction and good compatibility are evaluated to remarkably increase the miscibility and mechanical interlocking, ultimately enhancing the thermal conductivity, mechanical and tribological properties. Therefore, the PEI-BNO sizing layer on CF has proven to have great potential for high-performance CF/PEEK composites. [Display omitted] [ABSTRACT FROM AUTHOR]