A chemical looping (CL) reactor can provide the energy required to produce syngas from the reforming of glycerol. This can be done through the dynamic operation of packed-bed (PB) reactors that consecutively cycle in a three-stage process that includes oxidation, reduction, and a reforming stage. In this work, Ni-/Fe-based materials were synthesized, characterized, and tested as oxygen carriers and glycerol reforming catalysts during chemical looping reforming in packed-bed (CLR-PB) reactors. Two materials were prepared via coprecipitation/impregnation with different Ni loads (4.3 and 12 wt %) and similar Fe loadings (9.9 and 8.5% wt) and later on granulated to produce particles in a size cut of 0.6−1 mm. The materials presented high catalytic activity in a wide range of reforming temperatures (650−800 °C), being able to achieve over 95% glycerol-to-gas molar conversion in very short gas/solid contact times and at relevant conditions suitable for process scale-up. The results indicated that it is possible to produce materials with a low Ni load, which present sufficient catalytic activity and thermochemical capacity thanks to the presence of Fe, to operate under the glycerol CLR-PB configuration.