It is of utmost importance to optimise and stabilise hydrogen storage capacity during multiple cycles of hydrogen release and uptake to realise a hydrogen-based energy system. Here, the direct solvent-based synthesis of magnesium hydride, MgH 2 , from dibutyl magnesium, MgBu 2 , in four different carbon aerogels with different porosities, i.e., pore sizes, 15 < D avg < 26 nm, surface area 800 < S BET < 2100 m 2 /g, and total pore volume, 1.3 < V tot < 2.5 cm 3 /g, is investigated. Three independent infiltrations of MgBu 2 , each with three individual hydrogenations, are conducted for each scaffold. The volumetric and gravimetric loading of MgH 2 is in the range 17 to 20 vol % and 24 to 40 wt %, which is only slightly larger as compared to the first infiltration assigned to the large difference in molar volume of MgH 2 and MgBu 2 . Despite the rigorous infiltration and sample preparation techniques, particular issues are highlighted relating to the presence of unwanted gaseous by-products, Mg/MgH 2 containment within the scaffold, and the purity of the carbon aerogel scaffold. The results presented provide a research path for future researchers to improve the nanoconfinement process for hydrogen storage applications.