Homo- and heterodinuclear Yb/Yb and Gd/Gd or Yb/Al and Gd/Al helicates are obtained from 8-hydroxyquinoline-derived ligands and metal ions in a potassium-templated self-assembly process. X-ray structural investigations reveal an unusual pi-type coordination of the template to a vinylic unit. The compounds show high stability in solution and efficient NIR emission.