The selective metallization of nonconductive polymer materials has broad applications in the fields of integrated circuit technology and metallized patterns. This work discusses a methodology to pattern metal tracks on polybutylene terephthalate substrates. The process consists of three steps: 1) surface patterning with picosecond laser pulses (1030 nm) in air, 2) Pd seeding via treatment in PdCl2 solution, and 3) selective metallization via electroless copper deposition. Picosecond laser irradiation promotes not only surface roughening but also chemical modification to enable Pd seeding as the polymer surface acquires the ability to reduce Pd(II)‐chloride species to metallic Pd. The laser parameters, as well as the PdCl2 concentration and seeding temperature, have an influence on the polymer surface morphology, the concentration and distribution of metallic Pd, and the copper layer properties. Homogeneous copper layers with well‐defined geometries, good coating‐substrate adhesion, and high electrical conductivity can be obtained. This is ascribed to the synergistic effect of the chemical surface activation and roughness development (from 0.13 to ≈1.6 μm). As the patterning and surface activation are performed in air, directly on the as‐received polymer substrate, this methodology shows great potential for metallization of electronic devices with 3D complex geometries.