%0 Journal Article %T Selective Synthesis and Structural Transformation of a 4-Ravel Containing Four Crossings and Featuring Cp*Rh/Ir Fragments. %A Dang LL %A Zhang TT %A Chen T %A Zhao Y %A Gao X %A Aznarez F %A Ma LF %A Jin GX %J Angew Chem Int Ed Engl %V 62 %N 20 %D May 2023 8 %M 36929534 %F 16.823 %R 10.1002/anie.202301516 %X Intricately interwoven topologies are continually being synthesized and are ultimately equally versatile and significant at the nanoscale level; however, reports concerning ravel structures, which are highly entwined new topological species, are extremely rare and fraught with tremendous synthesis challenges. To solve the synthesis problem, a tetrapodontic pyridine ligand L1 with two types of olefinic bond units and two Cp*M-based building blocks (E1, M=Rh; E2, M=Ir) featuring large conjugated planes was prepared to perform the self-assembly. Two unprecedented [5+10] icosanuclear molecular 4-ravels containing four crossings were obtained by parallel-displaced π⋅⋅⋅π interactions in a single-step strategy. Remarkably, reversible structural transformations between the 4-ravel and the corresponding metallocage could be realized by concentration changes and solvent- and guest-induced effects. X-ray crystallographic data and NMR spectroscopy provide full confirmation of these phenomena.