Methylene blue (MB) is a refractory organic pollutant that poses a potential threat to the aquatic environment. Fenton reaction is considered a primrose strategy to treat MB. However, the traditional Fenton process is plagued by narrow pH application range, poor stability, and secondary pollution. To solve these problems, many Fenton-like catalysts including metal-organic frameworks (MOFs) have been prepared. Herein, a novel bimetallic MOF (Fe/Ce-BDC@CS) was prepared through simple adsorption for the effective removal of MB, where chitosan (CS) was used as the carrier. The degradation performance of Fe/Ce-BDC@CS (100 % within 20 min) was better than that of most reported monometallic MOFs. Moreover, Fe/Ce-BDC@CS exhibited good repeatability and its anti-interference performance of some inorganic ions was also remarkable. Column loading experiments showed that the removal efficiency of MB was still about 50 % over 155 h with a flowing speed of 0.30 L/h. Comparative analysis indicated that such excellent performances could be attributed to the synergistic effect between Fe and Ce. Furthermore, the results of quenching tests indicate that OH, O2−, and 1O2 contributed to MB degradation. In brief, Fe/Ce-BDC@CS has promising prospects in MB treatment, which can provide scientific references for the design and application of bimetallic MOFs.