Surface modification of Ar plasma-pretreated high density polyethylene (HDPE) film via UV-induced graft copolymerization with glycidyl methacrylate (GMA) and 2-hydroxyethylacrylate (HEA) was carried out to improve the adhesion with evaporated copper. The surface compositions of the modified HDPE surfaces were characterized by X-ray photoelectron spectroscopy (XPS). The adhesion strengths of evaporated copper with the graft-copolymerized HDPE films were affected by the Ar plasma pretreatment time, the monomer concentration used for graft copolymerization, and the graft concentration. Post-treatments, such as plasma post-treatments after graft copolymerization and thermal treatment (curing) after metallization, further enhanced the adhesion strength of the Cu/HDPE laminates. The T-type peel strengths of the laminates involving the graft-modified and plasma posttreated HDPE films were greater than 15 N/cm. The enhanced adhesion strength resulted from the strong affinity of the graft chains for Cu and the fact that the graft chains were covalently tethered on the HDPE surface. XPS characterization of the delaminated surfaces of the Cu/HDPE laminates revealed that the failure mode of the laminates with T-peel adhesion strengths greater than 5 N/cm was cohesive in nature.