AbstractCucurbituril homologues are multi‐functional macrocycles that can find applications in many areas and have numerous interesting features setting them apart from the other macrocycles. Among them, the ability of one of the cucurbituril homologues, cucurbit[6]uril (CB6), to catalyze 1,3‐dipolar cycloaddition in a regiospecific fashion is truly exceptional. Using this feature, small molecules can be clicked together to form complex structures in a very efficient way. Accordingly, in this article we review recent research involving the use of CB6‐catalyzed 1,3‐dipolar cycloaddition or the click reaction of CB6 in the construction of supramolecular assemblies including rotaxanes, pseudorotaxanes, polyrotaxanes, polypseudorotaxanes, molecular switches, machines, and nanovalves.