Catalytic decomposition of methane is a more sustainable alternative for hydrogen production compared to established technologies like steam methane reforming and coal gasification. This study reports iron-based catalysts supported on MAl2O4 (M = Ca, Mg, Sr, Ba) prepared via a ball-milling or one-pot modified Pechini (sol-gel) method. The synthesized catalysts were evaluated for their CDM performance in the range of 750-800°C. In general, we show that ball-mill synthesis leads to higher CDM activities than sol-gel synthesized samples which undergo quick deactivation. Raman spectroscopy and H2-TPR indicate that synthesizing the Fe-MAl2O4 catalysts via the sol-gel method results in iron coordination with cations (i.e. M) and with alumina to decrease iron’s reducibility and its overall catalytic activity. For the ball-mill synthesized samples, we find that a 30wt% Fe-CaAl2O4 catalyst tested at optimized reaction conditions of Tred = 700°C, Trxn = 750°C, yCH4 = 0.9, and GHSV = 1.25 L·g-1·h-1 obtained a competitive carbon yield of 17.86gC/gFe (5.06gC/gCat). TEM and SEM of the spent product indicate that the carbon product forms primarily via a tip-growth mechanism, with both filamentous and nano-onion type carbon being generated. Raman spectroscopy of the spent product determined most of the carbon formed on the ball milled Fe-MAl2O4 catalysts was graphitic in nature with ID/IG ratios ranging between 0.400-0.500. Overall, ball-milling appears to be a simple yet effective strategy to prepare dispersed iron catalysts for CDM.