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Introduction of atropisomeric axes into a bent bispyridine ligand leads to the quantitative formation of a complex mixture of atropisomeric M 2 L 4 cages upon treatment with metal ions. Whereas the isomer ratio of the obtained cage mixture, consisting of up to 42 isomers, is insensitive to temperature and solvent, the quantitative convergence from the mixture to a single isomer is accomplished upon encapsulation of a large spherical guest, namely fullerene C 60 . The observed isomerization with other guests depends largely on their size and shape ( e.g. , <10 and 82% convergence with planar triphenylene and bowl-shaped corannulene guests, respectively). Besides the unusual guest-induced convergence, the present cage mixture displays the strongest guest emission ( Φ F = 68%) among previously reported M n L m cages and capsules, upon encapsulation of a BODIPY dye in water., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)