Triangular triscatechol ligands are prepared in facile reaction sequences. The catechol units are either bound to the triangular backbone through their 3- or 4-position. With titanium(IV) ions, the ligands form metallosupramolecular M4L4 tetrahedra which are characterized by ESI MS and proton NMR. Quantum-chemical calculations reveal that connectivity at the catechol in the 3-position results in highly condensed structures while attachment in the 4-position affords container molecules providing huge internal cavities.