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To develop multifunctional protein imprinted materials, a cobalt-iron double ion-BSA directional chelation-assisted thermo-sensitive surface-imprinted hollow nanocage (Co-Fe@CBMA-MIPs) with excellent specificity is developed on the surface of ZIF-67@Co-Fe in this study by synergizing the advantages of surface imprinting, metal ion chelation, anti-protein adsorption segments, and thermo-sensitive components. Beyond previous research, well-designed multifunctional protein-imprinted materials possess high binding capacity, fast adsorption kinetics, and outstanding selectivity. When the adsorption is carried out at 32 °C, the adsorption capacity of Co-Fe@CBMA-MIPs for BSA reaches 520.35 mg/g within 50 min. The imprinting factor is 8.55. The selectivity factors of Co-Fe@CBMA-MIPs for HSA, Bhb, OVA, and Lyz are 3.72, 6.09, 4.10, and 8.41, respectively. More significantly, Co-Fe@CBMA-MIPs could specifically recognize BSA from mixed proteins and actual samples and exhibit excellent repeated use stability. Based on the above advantages, the development of this research provides an effective means to improve the recognition specificity of molecularly imprinted polymers.