Scientists are currently more interested in carbon allotropes since they are still having significant challenges in employing metal hydrides to achieve high hydrogen storage capacities. Mg–Ti alloy was created via mechanical alloying with MWCNT added. XRD confirms that the Mg–Ti solid solution exists. The existence of carbon in the Mg–Ti alloy was further validated by Raman analysis. The TEM investigation reveals that the electron diffraction measurements for the samples prior to hydrogenation have d spacing values of 2.3, 1.44, and 1.0,. The corresponding planes for these values are the (103) and (201) planes of the Mg–Ti intermetallic alloy of the FCC phase, as well as the CNTs plane of (002). In thermal analysis, as the exothermic peak dropped from 355.1 °C to 346 °C, in the same way that the activation energy dropped from 277.38 kJ/mol to 82.7 kJ/mol. The cyclic voltammetry examination of the Mg–Ti alloy with 4 wt% MWCNT added reveals a distinct anodic peak at −0.54 V. The calculated Cdl value for the Mg67Ti29MWCNT4 alloy in the impedance spectroscopy investigation is 2.372 F. Following the addition of MWCNT to the Mg–Ti alloy, the CR rate similarly decreased from 0.1728 to 0.1614 mgpy. Higher absorption capacity of 815 mAhg−1 and very long stable cycle life is demonstrated by the 4 wt% MWCNT added Mg–Ti.