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Nowadays, hydrogen has a preponderant position among the potentially sustainable energy sources. Due to its power density, its storage is of main concern when considering a broad use in practical applications. Carbon nanotubes constitute promising candidates for the design and construction of hydrogen storage devices. This work explores the use of some procedures involving electrochemistry, aimed to bond atomic Ti on the outer surface of MWNTs. Each titanium atom has the potential of hosting two hydrogen molecules and relinquishing them by heating. Nevertheless, nanotubes are difficult to handle due to electrostatic charge and agglomeration, and in this context, two routes were tested as procedures to spread and stick nanotubes on an electrode: (1) a functionalization capable of attaching gold was tested in two forms, as either using 4 nm particles or a flat gold electrode. The fixation of Au particles was confirmed by HRTEM. (2) A simpler route that consisted on drying a CH2Cl2/nanotubes solution previously spread on a glassy carbon flat electrode. CH2Cl2 was selected as the medium and TiCl4 as the precursor for attaching atomic Ti to the nanotubes. The results revealed that hydrogen adsorption, estimated from voltamperometry, was five times higher on Ti-MWNTs than on bare nanotubes.