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Interface issues urgently need to be addressed in high-performance fiber reinforced composites. In this study, different periods of O2 plasma treatment are proposed to modify twist-free polyimide (PI) filaments to improve hydrophilicity and mechanical and interfacial properties. Feeding O2 produces chemically active particles to modify the filament surface via chemical reactions and physical etching. According to the X-ray photoelectron spectroscopy (XPS) results, the PI filaments exhibit an 87.16% increase in O/C atomic ratio and a 135.71% increase in the C–O functional group after 180 s O2 plasma treatment. The atomic force microscope (AFM) results show that the root mean square roughness (Rq) of the treated PI filaments increases by 105.34%, from 38.41 to 78.87 nm. Owing to the increased surface oxygenic functional groups and roughness after O2 plasma treatment, the contact angle between treated PI filaments and water reduces drastically from the pristine state of 105.08° to 56.15°. The O2 plasma treated PI filaments also demonstrate better mechanical properties than the pristine PI filaments. Moreover, after O2 plasma treatment, the adhesion between PI filaments and poly(amic acid) (PAA) is enhanced, and the tensile strength of the polyimide/poly(amic acid) (PI/PAA) self-reinforced composites increases from 136 to 234 MPa, even causing the failure mode of the composite changes from adhesive failure to partly cohesive failure. [ABSTRACT FROM AUTHOR]