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The assembly of molecular Borromean Rings from con- stitutionally independent rings in a stepwise manner depends on the preparation of robust "ring-in-ring" complexes. The π-electron rich macrocycle bis-1,5-dinaphtho(50)crown-14 (1) is shown to form a donor-acceptor ring-in-ring complex with the π-electron poor cyclo- phane cyclobis(paraquat-4,4'-biphenylene) (2 4+ ) in solution. In the crystal superstructure of (1⊂2)·4PF6, CH···O interactions between the polyether loops of 1 and the bipyridinium units of 2 4+ could disfavor

Towards the Stepwise Assembly of Molecular Borromean Rings. A Donor-Acceptor Ring-in-Ring Complex