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Carbon nanotube (CNT)-reinforced 6061Al alloy matrix composites were prepared by chemical vapor deposition (CVD) combined with hot extrusion technique. During the preparation process, the 6061Al flakes obtained by ball milling of the 6061Al spherical powders were subjected to surface modification to introduce a hydrophilic polyvinyl alcohol (PVA) membrane on their surface (6061Al@PVA) to bond strongly with nickel acetate [Ni(II)]. Then the 6061Al@PVA flakes bonded with Ni(II) were calcined and reduced to Ni nanoparticles, which were then heat-treated at 580 °C to remove PVA for obtaining even Ni/6061Al catalyst. After that, the as-obtained Ni/6061Al catalyst was employed to synthesize CNTs on the surface of the 6061Al flakes by CVD. After hot extrusion of the CNT/6061Al composite powders, the as-obtained CNT/6061Al bulk composites with 2.26 wt% CNTs exhibited 135% increase in yield strength and 84.5% increase in tensile strength compared to pristine 6061Al matrix.