Microscopic deformation behavior is an important part of the study of micro-grinding processing. This paper investigates the removal mechanism in the micro-grinding of selective laser melting FeCoCrNiAl0.5 high-entropy alloy. The micro-grinding process is analyzed through simulation using the molecular dynamics simulation method. The study examines how the thickness of the undeformed chip and the grain size affect the microdeformation behaviors of shear strain, micro-grinding force, the evolution of dislocations, and microstructural transformation. The experimental results confirm that the molecular dynamics simulation model accurately predicts the micro-deformation behavior of FeCoCrNiAl0.5 high-entropy alloy during micro-grinding. The micro-deformation mechanism involves dislocation slip and twinning deformation, while the removal mechanism mainly includes the elimination of axial and dendritic crystals. During micro-grinding, the grinding force experiences small to large fluctuations, and the total length of dislocations gradually increases. As the undeformed cutting thickness increases, the micro-grinding force also gradually increases. Simultaneously, the type of dislocations and laminar dislocation nuclei increase, leading to growth in the total length of dislocations. The number of high shear strain atoms, the micro-grinding force, and the degree of fluctuation in the single crystal high-entropy alloy are higher than those in the polycrystalline material, but the total dislocation length is significantly smaller.