Here we investigate the synthesis of high-nuclearity heterometallic titanium oxo-alkoxy cages using the reactions of metal chlorides with [Ti(OEt)(4)] or the pre-formed homometallic titanium-oxo-alkoxy cage [Ti7O4(OEt)(20)] (A). The octanudear Ti7CoII cage [Ti7CoO5(OEt)(19)Cl] (1) (whose low-yielding synthesis we reported earlier) can be made in better yield, reproducibly by the reaction of a mixture of heptanuclear [Ti7O4(OEt)(20)] (A) and [KOEt] with [(CoCl2)-Cl-II] in toluene. A alone reacts with [(CoCl2)-Cl-II] and [(FeCl2)-Cl-II] to form [(Ti7CoO5)-O-II(OEt)(18)Cl-2] (2) and [(Ti7FeO5)-O-II(OEt)(18)Cl-2] (3), respectively. Like. 1, compounds 2 and 3 retain the original Ti-7 fragment of A and the II-oxidation state of the transition metal ions (Tm). In contrast, from the reaction of [Ti(OEt)4] with [(CrCl2)-Cl-II] it is possible to isolate [(Ti3CrO)-O-V(OEt)(14)Cl] (4) in low yield, containing a Ti3CrV core in which oxidation of Cr from the II to V oxidation state has occurred. Reaction of [(MoCl5)-Cl-V] with [Ti(OEt)](4) in [EtOH] gives the Ti8Mo4V cage [{Ti4Mo2O8(OEt)(10)}(2)] (5). The single-crystal X-ray structures of the new cages 2, 3, 4, and 5 are reported. The results show that the size of the heterometallic cage formed can be influenced by the nuclearity of the precursor. In the case presence of homometallic Mo-Mo bonding also appears to be a significant factor in the final structure.