Novel hierarchical metal-organic framework/chitosan aerogel composites were developed for oil bleaching. UiO-66-COOH-type metal organic frameworks (Zr-MOFs) were synthesized and integrated onto a chitosan matrix with different contents and named MOF-aerogel-1 and MOF-aerogel-2. Due to the compatibility of chitosan, the carboxylic zirconium MOF-aerogels not only maintained the inherent chemical accessibility of UiO-66-COOH, but the unique crystallization and structural characteristics of these MOF nanoparticles were also preserved. Through 3-dimensional reconstructed images, aggregation of the UiO-66-COOH particles was observed in MOF-aerogel-1, while the MOF was homogeneously distributed on the surface of the chitosan lamellae in MOF-aerogel-2. All aerogels, with or without immobilized MOF nanoparticles, were capable of removing carotenoids during oil bleaching. MOF-aerogel-2 showed the most satisfying removal proportions of 26.6%, 36.5%, and 47.2% at 50 °C, 75 °C, and 100 °C, respectively, and its performance was very similar to that of commercial activated clay. The reuse performance of MOF-aerogel-2 was tested, and the results showed its exceptional sustainability for carotenoid removal. These findings suggested the effectiveness of the MOFaerogel for potential utilization in oil bleaching treatments.