The surface properties of the AZ91D alloy are altered using surface mechanical attrition treatment (SMAT), a promising method of severe surface deformation, where the role of process parameters is crucial. In this study, specimens are SMATed using ≈3 and ≈10 m s−1 ball velocities (maintaining a constant percentage coverage). The SMATed specimens show higher twin density near the surface, which is reduced gradually, and twin thickness is increased with increasing depth. Further, high-velocity balls cause more twin density and better grain refinement (≈32 nm grain size at the surface). The higher ball velocity helps form a considerably thicker gradient layer (≈3500 μm) with higher hardness (≈1.98 GPa) and compressive residual stress (≈281 MPa) within a shorter SMAT duration (≈10 min). Ball velocity also influences nanomechanical properties such as nanohardness, creep resistance, strain rate sensitivity (SRS), etc. The non-SMATed alloy's SRS is about 0.037–0.040. The gradient microstructure affects SRS. The SRS value near the SMATed surface (where the reduced grain size plays a dominating role) is about 0.018–0.027; however, it drops suddenly to ≈0.01 (with a slight increase in depth), and subsequently, it rises with an increased distance in the SMATed layer (where twins play a dominating role).