This paper reports precision measurements of the electromagnetic permittivity of five highly refractive, singlecrystal materials, SrTiO 3 , KTaO 3 , rutile TiO 2 , LiTaO 3 , and LiNbO 3 , using a single, well-controlled, frequency-scalable procedure over the frequency ranges 25-110 and 140-220 GHz. Real permittivity values were highly consistent for different samples measured across multiple frequency bands. For SrTiO 3 , KTaO 3 , and TiO 2 , real permittivities were more consistent with lower frequency values than typically reported in the millimeterwave region of the spectrum. Real permittivities of LiTaO 3 and LiNbO 3 agreed with most reported data. The intrinsic dielectric loss of SrTiO 3 , KTaO 3 , and the extraordinary axis of rutile TiO 2 was also characterized over the ranges 25-110 and 140-220 GHz, and intrinsic loss per unit frequency was found to be consistent with values measured at other frequencies by dielectric resonators and quasi-optical techniques.