Cold sprayed polymer substrates offer a promising platform for bridging electroless deposition methods and applications. This study’s contribution to the field is the combination of cold sprayed polymer substrate and the electroless-plating process. In simulation, finite element analysis of the as-sprayed polymer substrate using a viscoelastic model that considers large strain time-dependent behavior were conducted. A three-network constitutive model was applied to capture the non-linear and time-dependent response of large strain polymer deformation. In experiment, the process-structure-property relationship was examined from the as-sprayed specimen to the final coated electroless-plated samples. A controlled coating process of Cu powders was first cold sprayed on polyamide 6. The as-sprayed specimen was then electroless deposited. Mechanical testing was performed on as-sprayed specimens and adhesion testing was performed on electroless deposited specimens. Scanning electron microscopy (SEM) was employed to observe the surface and the cross-section of the as-sprayed and electroless deposited specimens. Lastly, the behavior of Cu coated specimens immersed in KOH solution was examined by cyclic voltammetry.