The origin of the stray light appearing in the low wavenumber Raman spectra was studied on a double monochromator with a charge coupled device (CCD) detector by theoretical calculations and experimental observations. It is verified that the effect of the secondary maxima of the diffraction grating on the spectrum cannot be ignored, and the secondary maxima of Rayleigh scattering lead to the stray light in low wavenumber Raman spectra. The dependence of operating parameters for a double monochromator with a CCD detector working in the additive mode on the spectral feature has been calculated and experimentally observed. This may give a quantitative suggestion for proper choice of operating parameters that can efficiently suppress stray light in low wavenumber Raman spectra. Copyright © 2011 John Wiley & Sons, Ltd.