Light absorption and reflectance by smectite clays containing various adsorbed ions were measured in the UV, VIS, and NIR ranges and compared to Martian dust and surface soil spectra. Structural iron in the octahedral sheet of smectites is responsible for a characteristic absorption feature in the UV at 240--260 nm, resulting from an O2→Fe3+ charge transfer that is similar to one observed in the Martian spectrum. Adsorbed iron affects, via crystal field absorptions, the reflectance of montmorillonite in the VIS and NIR (to 1.3 μm), causing stronger absorption and higher opacity in the wavelength range 0.4--0.6 μm, without developing any specific pronounced absorption feature. In both general appearance and presence of, or lack of, spectral features, the iron-montmorillonite reflectance spectra in the VIS and NIR are similar to the Martian spectra. At present, however, spectral similarity cannot be used as the sole criterion for constraining Martian mineralogy since several other minerals, other than Fe-smectites, show sufficient similitude to the Martian spectra; other properties have to be explored and combined to obtain a definitive identification.