To study the influence mechanisms of tool geometry parameters on surface quality and subsurface damage when nanocutting polycrystalline NiFeCr superalloys, based on the theory of molecular dynamics, a three-dimensional nanocutting model is established. By investigating the mechanisms of material removal, cutting force, friction coefficient, surface roughness, residual stress, dislocation density, and phase transformation atoms, the influences of the tool rake angles, edge radii, and clearance angles on the surface and subsurface structures are analysed in detail. At the initial cutting stage, the material removal mechanism is dominated by tool extrusion, and as cutting continues, the dominant removal mechanism transforms into shearing. When the tool rake angle changes from negative to positive, the surface roughness improves, the dislocation density and phase transformation atoms decrease, and the tensile residual stress increases. As the edge radius increases, the surface roughness and dislocation density increase, the tensile residual stress decreases, and the phase transformation atoms first increase and then decrease. With the increased tool clearance angle, the surface roughness and phase transformation atoms decrease, the tensile residual stress increases first and then decreases, and the dislocation density shows fluctuating characteristics. In addition, an analysis of dislocation and defect evolution reveals the plastic deformation and subsurface damage mechanisms during nanocutting. In particular, grain boundaries help to inhibit the proliferation of defect damage and dislocations, and the interactions of dislocations form new dislocations. [ABSTRACT FROM AUTHOR]