We exploit epitaxial relationships of rutile-type VO2 with (0001) Al2O3, (111) LaAlO3, (10‾10) Al2O3, and
(10‾12) Al2O3 to achieve high-quality VO2 thin-film synthesis. We show that the deposition temperature can be lowered when these substrates are employed compared to one with no preferred crystallographic relationship with VO2, such as Si. We also report the first thin-film synthesis of the metastable VO2(B) polymorph on (001) LaAlO3 with a strongly preferred (001) out-of-plane orientation. These results are of interest for integrating VO2 films with other oxides in optoelectronic and reconfigurable device structures.