Laser shock peening (LSP) is a mechanical surface treatment process to modify near-surface material properties. Compared to conventional shot peening (SP) the process parameters can be finely adjusted with greater precision and a higher penetration depth of compressive residual stresses could be reached. However, high process times of LSP leads to high production costs. In this study, ultrafast LSP (U-LSP) with an ultrafast laser source (pulse time in the picosecond range) was applied on specimens made of X5CrNiCu15-5 and AlZnMgCu1.5. The surface characteristics (surface roughness) and surface-near properties (microstructure, residual stresses, and phase composition) were compared to the as-delivered condition, to conventional laser shock peening (C-LSP), and to SP, whereas metallographic analyses and X-ray and synchrotron radiation techniques were used. The process time was significantly lower via U-LSP compared to C-LSP. For X5CrNiCu15-5, no significant compressive residual stresses were induced via U-LSP. However, for AlZnMgCu1.5, similar compressive residual stresses were reached via C-LSP and U-LSP; however, with a lower penetration depth. A change in the phase portions in the surface layer of X5CrNiCu15-5 after C-LSP compared to SP were determined.