AbstractGrinding could be used to enhance accuracy and quality of carbon fiber‐reinforced poly‐ether‐ether‐ketone (CF/PEEK) composites. However, the grinding mode, namely up‐grinding (UG) or down‐grinding (DG), is usually neglected while unbefitting grinding mode choice may cause inferior surface quality. To investigate effects of grinding modes on grinding performance of anisotropic CF/PEEK, grinding experiments in UG and DG were carried out under different fiber orientation angles θ. Experimental results indicated that maximum grinding temperatures and normal grinding forces in UG were lower than DG regardless of the abrasive grit sizes. Material removal mechanisms of CF/PEEK affected by grinding mode were revealed by analyzing morphologies of surface, chip and grinding wheel. When θ = 0°, the dominant mechanisms in DG were extrusion fracture and fiber deformation, while they were interface shear debonding and bending fracture in UG. When θ = 90°, the dominant mechanisms in DG included interface layer separation and bending fracture, while they were shear and extrusion fracture of well‐supported fibers in UG. Thus, UG was more favorable for material removal, obtaining lower surface roughness values, fewer machining defects and less wheel wear than DG. This study will provide technical guidance for high‐quality grinding of carbon fiber‐reinforced thermoplastic composites.Highlights The effects of grinding modes (DG and UG) on the grinding performance of anisotropic CF/PEEK composites were investigated. Material removal mechanisms of CF/PEEK affected by grinding mode were revealed under different fiber orientation angles. The maximum grinding temperatures and normal grinding forces in UG were lower than DG. UG was more favorable for material removal in grinding, and could produce better ground surface quality than DG.