Coal chemical looping gasification (CLG) using inexpensive oxygen carrier (OC) is a promising technology to obtain H2-rich syngas, and the OCs of copper/iron ore composite with an autothermal capability and red mud have been screened as the potential candidates in our previous investigation. However, the detailed synergetic effect between copper ore and iron ore, and the effect of reaction conditions on syngas production at different reactor scales are still unclear. In this work, the synergetic effect between copper ore and iron ore in composite OCs with different mixing ratios are detailedly investigated through H2 temperature-programmed reduction (TPR) tests. The results indicate that the copper ore addition can contribute the reduction of iron ore and form a new phase of CuFe2O4 between CuO in the copper ore and Fe2O3 in the iron ore, meanwhile observing the composite OC of Cu20Fe80@C generating a stronger synergetic effect in comparison to adjencent OCs. Moreover, the optimization of reaction conditions are conducted in a batch fluidized bed reactor (BFBR) by regulating the temperature, oxygen to fuel (O/F) ratio, and steam concentration for the Cu20Fe80@C and red mud OCs. It is found that a higher temperature is conducive to improving the coal conversion and syngas yield on the whole, but not the H2-rich syngas production. While a lower O/F ratio favors the preparation of H2-rich syngas, and the optimal steam concentration is determined as 50 vol% for both OCs under comprehensive consideration of gasification time, syngas yield and heating cost. Additionally, the copper/iron ore composite OC with excellent CLG performance and bed stability is further confirmed in a semi-continuous fluidized bed reactor (SFBR), which shows the effects of temperature and O/F ratio on syngas production similar to those in BFBR. In summary, the promising copper/iron ore composite OC exhibits good adjustability and adaptability for CLG process in terms of reaction conditions and reactor scales, respectively.