The highest mobility InSb epilayer grown to date by organometallic vapor phase epitaxy has been achieved by utilizing high-purity organometallic sources, choosing a reactor geometry to reproducibly control the source concentrations above the substrate, and using a high-integrity reactor system. On a p-type InSb substrate, an unintentionally doped layer had a 77 K n-type carrier concentration and mobility of 1.4 X 10(15) cm-3 and 2.53 X 10(5) cm2/V s. Growths on GaAs substrates were greatly affected by the lattice mismatch and had 77 K carrier concentrations similar to the InSb case but with mobilities of (5.0-9.0) X 10(4) cm2/V s. The crystal quality, morphology, and cyclotron resonance characteristics are reported and found to be comparable to state-of-the-art molecular beam epitaxy layers.