Tri-reforming methane with CO 2 , O 2 , and H 2 O mixtures requires a delicate balance of dry-reforming, partial oxidation, and steam-reforming reactions to improve the CO 2 conversion and H 2 /CO ratio. Nickel−alumina has been reported before for the tri-reforming of methane, although at higher temperatures (>900 °C). This is because the current approaches for nickel−alumina synthesis are ineffective in generating stronger catalyst−support interactions necessary to maintain higher active sites and stall carbon nanotube (CNT) deposition. Here, we report a synthesis method that allows controlled loading of nickel on alumina-based MIL-53 metal−organic framework followed by calcination to generate 2.5−10 wt % nickel nanoparticles dispersed on alumina. The 5 wt % nickel−alumina mixtures resulted in nanometer-sized crystallites, better metal dispersion, and more active sites for enhanced catalytic activity. This optimal loading of nickel allows stronger interaction with alumina for over 100 h of stable performance of tri-reforming at 800 °C, achieving ∼98% CH 4 conversion, ∼36% CO 2 conversion, and no carbon deposition while producing Fischer−Tropsch-ready feed containing a H 2 /CO ratio of 3.2.