Fe-based oxygen carriers (OCs) are widely used in chemical looping steam reforming (CLSR) due to excellent resistance to carbon buildup, low toxicity, and high activity. In this study, a type of nano NiO-Fe 2 O 3 /Al 2 O 3 Fe-based OC that can easily be reduced by fuels and re-oxidized by air was developed for use in glycerol CLSR. It was synthesized by co-precipitation and impregnation. Based on the quadratic regression orthogonal model, a quadratic polynomial function was established to investigate the effects of temperature ( T ), water/carbon ratio ( S / C ), and loading ( M ) on hydrogen content (HL) and hydrogen selectivity ( S ). The OCs were characterized by XRD, XPS, SEM/EDX-mapping, TEM, and H 2 -TPR to determine their physicochemical properties. XPS shows the Fe phase highly interacted with the Al 2 O 3 supporting matrix by forming Fe aluminates in NiO-Fe 2 O 3 /Al 2 O 3 . The S (85.33%) and HL (78.41%) were obtained under the optimal conditions T = 600 °C, S / C = 1.0 mol mol -1 and M = 0. A hydrogen content fluctuation within 4% was obtained under T = 700 °C, S / C = 1.0 mol mol -1 , and M = 2.5%, which means the cycle stability is perfect because of the addition of Ni. This study provides a basis for the development of efficient oxygen carriers in the CLSR system.