A conventional solution‐based route to a cyclic trimeric organozinc compound [{Zn(Et)(β‐diketonate)}3] (β‐diketonate=OC(OMe)CHC(Me)O, 1) is described, with 1 structurally characterized for the first time. The ligand selection of bidentate β‐diketonates is shown to be key to isolating a cyclic trimer. Additional reaction of β‐diketonates with diethyl zinc were spectroscopically characterized as compounds of the type [{Zn(Et)(β‐diketonate)}n] (β‐diketonate=OC(Me)CHC(Me)O, 2, OC(OtBu)CHC(Me)O, 3). Further studies have shown that selective oxidation of these species produces cubanes of the general formula [{Zn(OC(R)CHC(Me)O)2Zn(Et)OEt}2] (R=OMe, 4; Me, 5; OtBu, 6), allowing a high oxygen content whilst remaining structurally suitable for use as precursors. The successful deposition of thin films of zinc oxide through aerosol‐assisted chemical vapor deposition (AACVD), using a novel precursor, is described and fully characterized.