The work aims to achieve efficient and nondestructive removal of organic coatings on the surface of automotive carbon fiber reinforced resin matrix composites (CFRP) structural parts. In this work, recyclable melamine plastics were selected to prepare abrasives. A new machining method with air jet carrying and high-speed jetting was proposed. The polyurethane-coated CFRP specimens were eroded by single-factor control of the erosion angle with 500 μm abrasive at different erosion angles under 0.3 MPa jet pressure. The erosion morphology was observed with an SEM and a super depth-of-field 3D microscopy. The coating removal mechanism was illustrated by developing a micro cutting and repetitive deformation model based on the law of energy conservation. The particle velocity and contact stress, and quantitatively calculating the mass of coating loss were analyzed. The effects of abrasive shape, rotation and rebound on erosion mechanism were investigated. The results showed that the material removal rate of the coating was the largest when the erosion angle was 30°, and the removal rate was 5.8×104 g/s, which showed ductile erosion behavior, and the erosion mechanism was micro-plowing and micro-cutting at this time. The material removal rate decreased with the increase of the erosion angle, and when the erosion angle was 90°, the removal rate was 1.2×104 g/s. The erosion mechanism of the coating was repeated plastic deformation removal. Sharp angular particles impacted the coating with concentrated stress and removed the material in the form of cutting at the inclined angle. Whereas abrasives evolved from sharp angles to sub-spherical particles due to wear (which can be cycled 15 times) and impacted the coating with distributed stress. In addition, the removal of coatings by abrasives reverse rotation was greater than that of forward rotation attributed to the reverse rotation increasing the effective cutting speed. Large particle size rebound produced incomplete cutting paths and small particle size rebound produced tearing of the coating. In order to achieve non-destructive removal of substrate materials, it is recommended to use high erosion angle so as to retain primer and achieve non-destructive removal of substrate materials.