In this study, the interlaminar fracture toughness and impact strength of polyethersulfone reinforced with continuous carbon fibers were studied. Interlaminar fracture toughness tests were performed using the double cantilever beam method. It was shown that surface modification using the thermal oxidation method of the carbon fibers can strongly increase the interlaminar fracture toughness of the obtained composites. Thus, the maximum value reached 1.72 kJ/m2, which was 40% higher than the fracture toughness of the composites reinforced with initial carbon fibers. Moreover, fractographic analysis using a scanning electron microscope allowed us to highlight the main reasons for the dependence of fracture toughness on fiber content and surface modification conditions of the carbon fibers. It was shown that the main factor that allowed for an increase in fracture toughness was the enhanced interfacial interaction between the fibers and polymer matrix. Additionally, it was found that expectedly, there was a good correlation between interlaminar fracture toughness and interlaminar shear strength results. However, a negative influence of surface modification on the impact properties of composites was found. Such behavior occurred because of higher structural stability and lower exposure to delamination in multiple layers of the composites reinforced with the modified carbon fibers. It was found that impact energy reached ~150 kJ/m2 for the polyethersulfone-based composites reinforced with initial fibers, while the composites reinforced with modified carbon fibers showed impact energy values of only ~80 kJ/m2. Nevertheless, surface modification of carbon fibers using the thermal oxidation method can be an effective method for improving the performance properties of polyethersulfone-based composite materials.