We describe herein the self‐assembly synthesis of an octanuclear CoII [2]catenane {[Co4(H2L)6]216+} formed by the mechanical interlocking of two {[Co4(H2L)6]8+} rectangles of unprecedented topology. Subtle manipulation of the synthetic conditions allows the isolation of a mixed‐valence [Co2III/Co2II]10+ non‐catenated rectangle. The CoII centers in the [2]catenane exhibit slow relaxation of their magnetic moment, i. e. single‐molecule magnet properties, dominated by quantum tunneling and Raman relaxation processes. This work shows that metallo‐supramolecular chemistry can precisely control the organization of single‐molecule magnets in topologically complex arrangements.

We describe herein the self‐assembly synthesis of an octanuclear CoII [2]catenane {[Co4(H2L)6]216+} formed by the mechanical interlocking of two {[Co4(H2L)6]8+} rectangles of unprecedented topology. Subtle manipulation of the synthetic conditions allows the isolation of a mixed‐valence [Co2III/Co2II]10+ non‐catenated rectangle. The CoII centers in the [2]catenane exhibit slow relaxation of their magnetic moment, i. e. single‐molecule magnet properties, dominated by quantum tunneling and Raman relaxation processes. This work shows that metallo‐supramolecular chemistry can precisely control the organization of single‐molecule magnets in topologically complex arrangements.

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