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The infrared spectra of gaseous and liquid CH3OPCl2 and CD3OPCl2 have been recorded from 4000 to 33 cm− 1. The Raman spectra of the liquids have been recorded and depolarization values measured. No indication of a second conformer could be found in either the low-temperature Raman or infrared spectra. The interesting “methyl” torsion was observed at 127 cm− 1 for the hydrogen compound and 119 cm− 1 for the deuterium-containing molecule. Considerable mixing among the low-frequency skeletal modes and the torsional vibration was apparent. Assignment of the other fundamentals based on position, depolarization values, and isotopic shifts is given and discussed. It is shown that the band in the region of 1190-1170 cm− 1 which is characteristic of the CH3OP moiety results from a rocking motion of the methyl group rather than to a stretching motion of the COP group to which it is frequently assigned. The vibrations resulting from the COP group are better characterized as COP symmetric and COP antisymmetric stretching modes rather than C–O and P–O motions.