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Liquid crystal polymer (LCP) has potentially a very wide application as substrate material in electronic packaging applications because of its unique advantages. The work in this paper was performed to realize the metallization of LCP for the purpose of board fabrication, and to study the adhesion between deposited copper and LCP. A homogenous electroless plated copper layer on LCP with 4 to 5 μm thickness was achieved, while it increased up to 40 μm with the subsequent electroplating. The timescale of etching, deposit ion rate, and pH value were gradually changing during the plating process and the influences on copper layer quality were investigated. The adhesion force of the copper-LCP layer system was measured by a shear-off-method. Scanning electron microscopy (SEM) was used to check the surface morphology after etching and the interface after shearing on both the backside of the copper layer and the LCP side. The relationship between the shear-off adhesion of copper and the time of chemical etching before plating was examined, and the optimal etching time is discussed. Heat treatment after plating was used, and it was shown that this significantly improved the adhesion strength.