A new atomic layer deposition (ALD) process was applied for the uniform coating of carbon nanotubes with a number of transition-metal oxide thin films (vanadium, titanium, and hafnium oxide). The presented approach is adapted from non-aqueous sol-gel chemistry and utilizes metal alkoxides and carboxylic acids as precursors. It allows the coating of the inner and outer surface of the tubes with a highly conformal film of controllable thickness and hence, the production of high surface area hybrid materials. The morphology and the chemical composition as well as the high purity of the films are evidenced through a combination of electron microscopic and electron-energy-loss spectrometric techniques. Furthermore, in order to highlight a possible application of the obtained hybrids, the electrical and sensing properties of resistive gas sensors based on hybrid vanadium oxide-coated carbon nanotubes (V2O4-CNTs) are reported and the effect of thermal treatment on the gas sensing properties is studied.