<p>Carbon fiber-reinforced polymer (CFRP) has been widely utilized in aerospace and other fields due to its exceptional mechanical properties. However, the anisotropic and heterogeneous nature of this material poses significant challenges in its machining. Moreover, most research has focused on single layer and unidirectional CFRP, with limited studies on the material removal mechanisms of multilayer and multidirectional CFRP. The objective of this paper is to systematically characterize the surface damage of multilayer and multidirectional CFRP through conventional scratching (CS) and ultrasonic vibration-assisted scratching (UVAS) experiments using a single indenter, and to reveal the influence of different machining parameters on material removal behavior. The results indicate that the surface damage of multilayer and multidirectional CFRP caused by a single indenter primarily manifests as fiber fragmentation, fiber-matrix interface debonding, microscopic delamination, fiber fracture, fiber pull-out, and fiber shedding. Using an indenter with a smaller apex angle and scratching with the edge of the indenter are more conducive to fiber fracture and removal, with micro-delamination consistently occurring at the interface between two layers. As the scratching depth increases, fiber-matrix interface debonding intensifies. An increase in the exit angle enhances the compressive effect of the indenter, thereby reducing material removal efficiency. Ultrasonic vibration can shift the material removal mode from fiber fragmentation to fiber fracture, increase the width and depth of the scratch, effectively reduce the scratching force at large depths, but is prone to causing fiber pull-out phenomena.</p>