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High quality vertically aligned carbon nanotube (VACNT) arrays have been synthesized on bulk Al alloy (Al6063) substrates with an Fe catalyst using low pressure chemical vapor deposition (LPCVD). The pretreatment process of the catalyst was shown to play a critical role, and it was studied comprehensively and optimized to grow high quality VACNT arrays within a wide range thicknesses of catalyst layer (2nm - 11 nm) and acetylene (C2H2) flow rates (100sccm - 300sccm). The thermal performance of the resulting VACNT arrays is evaluated. The minimum thermal interfacial resistance of the Al-CNT-Si interfaces achieved so far is only 4 mm2·K/W, and the average value is 14.6 mm2·K/W.