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A facile and convenient approach for the synthesis of multi‐functionalized calix[4]arenes through multi‐component reactions is described. A series of five new calix[4]arene‐hexaamide derivatives were synthesized, and their structures were elucidated by means of spectroscopic data. The value of this method lies in its operational simplicity, mild reaction conditions, structural diversity of products, and good yields. Furthermore, fluorescence studies demonstrated considerable binding affinity of these new calix[4]arenes toward β‐lactoglobulin protein.

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