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Making full use of coordination‐driven self‐assembly strategy, we herein described the selective synthesis of a molecular Borromean rings and two cases of “U”‐shaped tweezer‐like molecular assemblies in high yield by using bipyridyl ligands based on biphenyl unit and half‐sandwich binuclear rhodium(III)/iridium(III) building blocks. The selective synthesis was realized by adjusting the length of dipyridyl...