Among the wide range of renewable energy sources, the ever-increasing demand for electricity storage represents an emerging challenge. Utilizing carbon nanotubes (CNTs) for energy storage is closely being scrutinized due to the promising performance on top of their extraordinary features. In this work, well-aligned multilayer carbon nanotubes were successfully synthesized on a porous silicon (PSi) substrate in a fast process using renewable natural essential oil via chemical vapor deposition (CVD). Considering the influx of vaporized multilayer vertical carbon nanotubes (MVCNTs) to the PSi, the diameter distribution increased as the flow rate decreased in the reactor. Raman spectroscopy results indicated that the crystalline quality of the carbon nanotubes structure exhibits no major variation despite changes in the flow rate. Fourier transform infrared (FT-IR) spectra confirmed the hexagonal structure of the carbon nanotubes because of the presence of a peak corresponding to the carbon double bond. Field emission scanning electron microscopy (FESEM) images showed multilayer nanotubes, each with different diameters with long and straight multiwall tubes. Moreover, the temperature programmed desorption (TPD) method has been used to analyze the hydrogen storage properties of MVCNTs, which indicates that hydrogen adsorption sites exist on the synthesized multilayer CNTs.