A method of incorporating both metal−ligand and crown ether−dialkylammonium self-assembly techniques in the efficient synthesis of metallacyclic tris[2]pseudorotaxanes is described. These multifunctional supramolecules can be prepared by the stepwise or one-pot assembly of nine separate components on account of the orthogonality of the two noncovalent assembly strategies employed. This methodology demonstrates the power of orthogonal self-assembly and may be expanded beyond the use of two recognition motifs in hopes of mimicking the complex multifunctionality of biological systems.