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In this work, we discuss the challenges associated with measuring and interpreting the vibrational properties of nanomaterials at mid- and far-infrared frequencies, where vibrational bands are often broad and overlapping. This issue is compounded by the complex interaction between infrared light and particulate samples, which depends on packing density and particle connectivity. Preliminary results concerning the far-infrared optical properties of Fe3O4 nanoparticles have been obtained using the two most reliable methods (specular reflectance and attenuated total reflectance). These results are compared to one another and to their Raman counterparts. Finally, the influences of particle size and composition on the vibrational spectra are qualitatively discussed. [ABSTRACT FROM AUTHOR]