Molecular knots have long been the subject of speculation. Now, for the first time, it has been possible to synthesize a “knotted” molecule having the topological chirality of a trefoil knot. Compound 1 was synthesized via a double-helix complex by exploiting the template effect of CuI ions. The chirality of 1 could be demonstrated by 1H NMR spectroscopy. The “unraveled” topological isomer of 1 was also synthesized.