A simple chemical solution process was used to prepare alumina nanoparticle-coated ZnO nanotubes (ANZTs). Transmission electron microscope (TEM) images proved that the alumina nanoparticles were uniformly dispersed on the ZnO nanotubes. After thermal treatment at different temperatures under various atmospheres, photoluminescence (PL) measurements showed that the ANZTs emitted a variety of colors, including blue, green and white light. Gaussian curve fitting of the PL spectra revealed that the competition between the blue, blue-green, green and yellow band emissions and their relative emission intensities were strongly associated with various defects. Blue emission was attributed to large numbers of oxygen defects in alumina, while green and yellow emissions were related to oxygen and zinc defects in ZnO, respectively. Under specific conditions, white light, consisting of blue, blue-green, green and yellow band emissions, was obtained. Further TEM analysis indicated that the defect structure of ANZTs could be manipulated by the interface interaction between alumina and the ZnO nanotubes.