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A lamination technique for liquid crystal polymer (LCP)/Cu was developed for high speed and high performance printed circuit boards (PCB). This approach was accomplished by using a modified surface activated bonding (SAB) process to achieve enhanced adhesion and a smooth interface. Systematic investigation of peel strength of four categories of samples, namely “as bonded”, “annealed”, “Cu-deposited”, and “Cu-deposited and annealed” showed highest peel strength in the “Cu-deposited and annealed” sample. Significant improvements in adhesion were observed in the samples cleaned with argon-radio frequency (Ar-rf) plasma (“as bonded” samples) followed by Cu deposition on LCP, which were heated after bonding in low vacuum pressure at 240°C (about 70–75 times higher than that of “as bonded”). XPS analyses on peeled surfaces of the “Cu-deposited and annealed” sample reveal bulk fracture in the LCP. Threefold lower loss in conduction of SAB processed laminate than that of conventional heat laminate was most likely due to smooth interface of the SAB processed laminate (surface roughness was ninefold lower than that of conventional heat laminate). A plausible adhesion mechanism of Cu/LCP might be due to bonding of Cu adhesion sites to plasma induced dangling sites of LCP surface, and thermal reconstruction of Cu deposited layers.