Two different types of carbon fibers (ultrahigh modulus and high strength carbon fibers) were surface-treated in an oxygen plasma under equivalent conditions. Changes in the fiber surface chemistry were followed by electrokinetic measurements (zeta potential). The oxygen plasma treatment resulted in a displacement of the isoelectric point of carbon fibers toward lower pHs, evidence of an increase in the surface acidity. The possible simultaneous formation of basic functional groups was also inferred and supported by results obtained by inverse gas chromatography and wettability measurements. Differences were more evident with ultrahigh modulus carbon fibers than with high strength carbon fibers. It is concluded that the measurement of the electrokinetic properties constitutes a useful technique to follow the evolution of the surface chemical characteristics of different types of carbon fibers.