Oxygen carrier (OC) particles for chemical-looping combustion (CLC) may be produced in large scale by a number of methods such as freeze granulation, spray drying, impregnation, and mechanical mixing methods. To select the most appropriate technology for large-scale preparation, the four preparation methods were adopted to prepare Fe2O3/Al2O3 OCs and compared with each other in terms of productivity, preparation period, physical and chemical characterization, and reactivity in CLC of lignite. Freeze granulation and spray drying methods were found to be more suitable for large-scale production of OCs for CLC. The results of the comparative studies may provide guidelines for selecting appropriate methods for preparing OCs on industrial scale.