Structural switching of [3]catenane was induced by fitting the puzzle pieces. In their Research Article (202217002), Jun Terao et al. report a method for ligand-controlled structural switching of [3]catenane, which was realized by the complexation of metal ions on [3]catenane with added complementarily fitted organic ligands, like pieces in a jigsaw puzzle. The high tailorability of organic ligands offers multiple pieces with various sizes and numbers of coordination sites, enabling multistate structural switching of [3]catenane. Structural switching of [3]catenane was induced by fitting the puzzle pieces. In their Research Article (202217002), Jun Terao et al. report a method for ligand-controlled structural switching of [3]catenane, which was realized by the complexation of metal ions on [3]catenane with added complementarily fitted organic ligands, like pieces in a jigsaw puzzle. The high tailorability of organic ligands offers multiple pieces with various sizes and numbers of coordination sites, enabling multistate structural switching of [3]catenane. Organic Electronics Carboranes Batteries Enzyme Catalysis