The effect of infrared (IR) irradiation on the immobilization of ZnO nanocrystals on the surface of functionalized carbon nanotubes (CNTs) is investigated. The hybrids are characterized by X-ray diffraction, infrared spectroscopy, X-ray photoelectron spectroscopy, and microscopy. The hexagonal wurtzite phase ZnO nanocrystals are formed on CNTs surface on calcination of the Zn(OH)2–CNT hybrids at 350 °C in a continuous flow of nitrogen. Microscopic measurements show that ZnO nanocrystals in size the range of 8 nm are formed when IR irradiation is employed; however, in the absence of IR irradiation, ZnO aggregates of the size of more than 100 nm are formed.