In this study, we adopted the chemical co-precipitation (CP) method and sol-gel method followed by calcination at temperatures of 100-900°C for 12h to synthesize CoFe2O4 materials, which were further characterized by TEM, XRD and XPS techniques. The properties of CoFe2O4 materials were evaluated in a microwave (MW) induced catalytic oxidation (MICO) process for the elimination of brilliant green (BG). The results showed that: (1) the removal rates of BG gradually decreased over a series of CoFe2O4 materials prepared by CP method and calcinated with 100-700°C (except 900°C) for 12h within three reuse cycles; for comparison, no removal of BG was obtained over CoFe2O4 synthesized by sol-gel method and CoFe2O4-900 (CP); (2) no hydroxyl radicals were captured with salicylic acid used as molecular probe in the MICO process; (3) MW irradiation enhanced the release of residual NaOH within the microstructure of CoFe2O4 and further discolored BG, because BG is sensitive to pH; (4) granular activated carbon (GAC), an excellent MW-absorbing material possessing higher dielectric loss tangent compared to that of a series of CoFe2O4 materials, could not remove BG in suspensions at a higher efficiency, even if the loading amount was 20 g L(-1). Accordingly, MICO process over CoFe2O4 materials and GAC could not effectively eliminate BG in suspensions.