Chemical looping methane reforming (CH4-CLR) is an advanced technology for syngas generation. However, the lack of suitable oxygen carrier (OC) materials is the main bottleneck restricting the industrialization of CH4-CLR. Current research has shown that inexpensive natural ilmenite ore is an ideal OC, however, it suffers from weak reactivity toward CH4, and the reaction between the two is easily inhibited by trace amounts of CO2. Here, the naturally occurring ilmenite ore has been used as both catalyst and OC in the CH4-CLR process. The reduced ilmenite ore (R-ilmenite) acts as a catalyst, activating CH4 and a small amount of CO2 in the feed gas, while the oxidized ilmenite ore (O-ilmenite) acts as an OC, partially oxidizing CH4 to generate syngas. The R-ilmenite catalyst and O-ilmenite OC are spatially distributed in the CH4-CLR reactor of fluidized beds to improve the reactivity of O-ilmenite toward CH4, catalyze CO2 conversion, and eliminate CO2 inhibition, as well as achieve the simultaneous CO2 utilization. Compared to the traditional method of improving the activity of ilmenite OC, this method fully utilizes the dual characteristics of cheap natural ore as both catalyst and OC, effectively overcoming the disadvantages of low activity and susceptibility to CO2 inhibition of iron-based OCs. This scheme not only greatly improves the performance of ilmenite OC, but also eliminates the need for significant chemical modification and physical treatment of the OC, nor does it require the introduction of guest components, thus improving the economy and practical operability.