The mechanical properties and stability of hydrophobic surface structures prepared by traditional methods are still the main technical bottlenecks restricting the broad application of hydrophobic systems on workpiece surfaces. In this contribution, we propose a technique called selective laser shock peening (SLSP) to enable large-scale high efficient, low-cost manufacturing of hydrophobic metal surfaces with enhanced mechanical properties for durable applications. Using the method of experimental investigation combined with numerical calculation, the hydrophobic properties, mechanical properties, and tribological properties of the samples prepared under SLSP, all-laser shock peening (ALSP), and non-laser shock peening (NLSP) are studied. The SLSP process could prepare a 3D gradient structure material with surface structures, a two-phase (strong phase, soft phase) distribution on the surface, and a multi-level gradient distribution in the thickness direction. Compared with the 2D gradient structure prepared by the traditional process, 3D gradient structures by SLSP have more significant advantages in improving the wetting behavior and the mechanical properties of the material, which proves SLSP to be a novel method to fabricate functional metal surface structures, with highly high engineering application value.