The growth of bamboo-like multiwalled carbon nanotubes (MWCNTs) over Cu/Al2O3 catalyst by chemical vapor deposition under atmospheric pressure using ethanol as the carbon source has been demonstrated. The obtained MWCNTs are dominant with bamboo-like morphology. The morphologies, graphitization degree, and microstructures of the products were characterized by transmission electron microscopy, X-ray diffraction, Raman spectroscopy, field emission scanning electron microscopy, high-resolution transmission electron microscopy, and selected area electron diffraction. The results show that the combination of Cu/Al2O3 catalyst and ethanol was critical for the growth of bamboo-like MWCNTs. The possible factors causing the formation of bamboo-like structures were also discussed.