The spectroscopic properties of hydrotalcite-like compounds, containing Co(II) and Fe(III) in the layers, have been studied. In these materials, depending on the experimental conditions during synthesis, Co(II) becomes partially oxidized to Co(III). Although the environment of the cations is close to octahedral in all cases, Mossbauer data indicate a more symmetric environment for Fe(III) ions in samples not submitted to hydrothermal treatment. The FT-IR spectra show some distortion of the carbonate anions in the interlayer space.