The reaction of [Ti-4(OMe)(14)Cl-2] (1) with an excess of AlMe3 gave the cocrystallite [Ti-2(mu-OMe)(2)(mu-Cl)Cl-3(thf)(3)].[Ti-2(mu-OMe)(3)Cl-3(thf)(3)] (2.3) species in a 1:1 ratio. Similar to 2, [Ti-2(mu-OEt)(2)(mu-Cl)Cl-3-(thf)(3)] (4) was obtained in the reaction of an equimolar mixture of TiCl4 and Ti(OEt)(4) with Al/AlMe3. The short distance [2.543(1)(av) Angstrom in 2.3 and 2.599(1) Angstrom in 4] between ''Ti(+3)'' atoms, their diamagnetism, and ELF analysis indicate the presence of a Ti-Ti bond.