Biogas plays a vital role in the emerging renewable energy sector and its efficient utilization is attracting significant attention as an alternative energy carrier to non-renewable fossil fuel resources. Since biogas consists mainly of CH 4 and CO 2 , dry reforming of methane arises as an appropriate process enabling its chemical conversion to high-quality synthesis gas (syngas: H 2 and CO mixtures). In this study, we synthesized via a direct "one-pot" method following an evaporation-induced self-assembly approach, ordered mesoporous Fe 10% , Ni 5% and Fe x% Ni (1-x) (x: 2.5, 5 or 7.5%) in Al 2 O 3 as catalysts for syngas production via dry reforming of a model biogas mixture (CH 4 /CO 2 ¼ 1.8, at a temperature of 700 o C). Monometallic Fe 10% Al 2 O 3 catalyst presented lower reactivity levels and slightly deactivated during catalysis compared to stable Ni 5% Al 2 O 3 . According to physico-chemical characterization techniques, the incomplete reduction of Fe 2 O 3 into Fe 3 O 4 rather than Fe 0 nanoparticles (catalytically active) coupled with the segregation of Fe 3 O 4 oxides were the main factors leading to the low performance of mesoporous Fe 10% Al 2 O 3 . These drawbacks were overcome upon the partial substitution of Fe by Ni (another transition metal) forming specifically bimetallic Fe 5% Ni 5% Al 2 O 3 displaying reactivity levels close to thermodynamic expected ones. The formation of Fe-Ni alloys stabilized iron inside alumina matrix and protected it from segregation. Along with the confinement effect, spent catalyst characterizations showed high resistance towards coke deposition.