The Self-Sorting Behavior of Circular Helicates and Molecular Knots and Links**

We report on multicomponent self-sorting to form open circular helicates of different sizes from a primary monoamine, Fe(II) ions, and dialdehyde ligand strands that differ in length and structure by only two oxygen atoms. The corresponding closed circular helicates that are formed from a diamine—a molecular Solomon link and a pentafoil knot—also self-sort, but up to two of the Solomon-link-forming ligand strands can be accommodated within the pentafoil knot structure and are either incorporated or omitted depending on the stage that the components are mixed.