In this study, coal gasification to produce synthesis gas by chemical looping was investigated with CuFe2O4 oxygen carriers (OCs), including the reaction characteristics and structural evolution process. It was found that the presence of a CuFe2O4 OC increases the gasification reaction rate of coal in comparison to the use of inert bed material (silica sand). The CuFe2O4 OC enhanced the performance of hematite and improved the ability to produce syngas of CuO OCs. During the chemical looping process, CuFe2O4 was reduced to Fe3O4 and Cu. Furthermore, N-2 adsorption/desorption and scanning electron microscopy images verified that the released O-2 and the generated CO2 by the CuFe2O4 OCs improved the carbon conversion and facilitated the pore opening and expansion shown by the increase in specific surface area. This can be used as a theoretical reference that can be used to gain a better understanding of the microscopic mechanism for how CuFe2O4 OCs can accelerate the chemical looping gasification of coal.