Reduced-graphene-oxide (rGO) aerogels provide highly stabilising, multifunctional, porous supports for hydrotalcite-derived nanoparticles, such as MgAl-mixed-metal-oxides (MgAl-MMO), in two commercially important sorption applications. Aerogel-supported MgAl-MMO nanoparticles show remarkable enhancements in adsorptive desulfurization performance compared to unsupported nanoparticle powders, including substantial increases in organosulfur uptake capacity (>100% increase), sorption kinetics (>30-fold), and nanoparticle regeneration stability (>3 times). Enhancements in organosulfur capacity are also observed for aerogelsupported NiAl-and CuAl-metal-nanoparticles. Importantly, the electrical conductivity of the rGO aerogel network adds completely new functionality by enabling accurate and stable nanoparticle temperature control via direct electrical heating of the graphitic support. Support-mediated resistive heating allows for thermal nanoparticle recycling at much faster heating rates (>700 °C•min −1) and substantially reduced energy consumption, compared to conventional, external heating. For the first time, the CO 2 adsorption performance of MgAl-MMO/rGO hybrid aerogels is assessed under elevated-temperature and high-CO 2-pressure conditions relevant for pre-combustion carbon capture and hydrogen generation technologies. The total CO 2 capacity of the aerogel-supported MgAl-MMO nanoparticles is more than double that of the unsupported nanoparticles and reaches 2.36 mmol•CO 2 g −1 ads (at p CO2 = 8 bar, T = 300 °C), outperforming other high-pressure CO 2 adsorbents.