Molecular beam epitaxy (MBE) growth of thin ($2 lm) CdTe layers characterized by high crystal quality and low defect density on lattice mismatched substrates, such as GaAs and Si, has thus far been difficult to achieve. In this work, we report the effects of in situ thermal deoxidation under In and As 4 overpressure prior to the CdTe growth on epiready GaAs(211)B wafers, aiming to enhance CdTe crystal quality. Thermally deoxidized GaAs samples were analyzed using in situ reflection high energy electron diffraction, along with ex situ x-ray photo-electron spectroscopy (XPS) and atomic force microscopy. MBE-grown CdTe layers were characterized using x-ray diffraction (XRD) and Everson-type wet chemical defect decoration etching. We found that In-assisted desorption allowed for easier surface preparation and resulted in a smoother surface compared to As-assisted surface preparation. By applying In-assisted thermal deoxidation to GaAs substrates prior to the CdTe growth, we have obtained single crystal CdTe films with a CdTe(422) XRD rocking curve with a full-width half-maximum value of 130.8 arc-s and etch pit density of 4 9 10 6 cm À2 for 2.54 lm thickness. We confirmed, by XPS analysis, no In contamination on the thermally deoxidized surface.