Improving methane catalytic decomposition process was deemed an effective approach for hydrogen production. Here, a novel catalyst AlxCo1-xFe2O4 with a variable aluminum content was synthesized via a co-precipitation route for the direct cracking of methane. The catalytic activity of AlxCo1-xFe2O4 was performed in a fixed bed reactor at temperature of 800 degrees C and 20 mL/min of fed gas. A sequence of characterizations, including SEM, BET, XRD, XPS, Raman and TGA for fresh and spent catalysts, was exploited to examine the influence of Al-x content on the morphology, porosity, structure, chemical composition, and cation distribution of AlxCo1-xFe2O4. As the Al-x content increased in AlxCo1-xFe2O4 their morphology became more fractal and decreased in particle size, lattice parameter, lattice size, while their pore surface increased. Further cation re-distributions from octahedral to tetrahedral sites as Fe3+ and Al3+ relocated in the Tetrahedral site and Oxygen lattice decreased as observed from Raman and XPS results. Catalytic activity studies showed that Al-x content of 0.6 in AlxCo1-xFe2O4 lead maximum methane conversion up to similar to 91.10 % and hydrogen formation rate of 1.780 x10(-3) mol H-2 g(-1) s(-1). The catalytic activity behavior was explained in correlation with the characteristics of spent catalysts.