Single-crystal (211) and (100) CdTe layers have been grown by metalorganic vapor-phase epitaxy using the same condition on (211) and (100) Si substrates, respectively. Prior to the growth, substrates of both orientations were pretreated using the same pretreatment procedure. The crystal qualities of the grown layers were evaluated by full-width at half-maximum values of double-crystal x-ray rocking curves, and photoluminescence spectra at 4.2 K. (211) CdTe layers showed better crystallinity than (100) layers. The crystal quality of the (100) CdTe layers was also compared with that of layers grown on an epitaxial (100) GaAs layer on Si substrate. The results suggest that (100) CdTe layers with improved crystal quality could be obtained by optimizing the procedure of the Si substrates.