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Assessment of random and systematic errors is performed for the first time on the real part of permittivity (ε') and loss tangent (tanδ) of ceramics and polymers using two different measurement systems. Data measured from the full cavity length and the frequency variation techniques using the 60 GHz open resonator system and the millimeter-wave dispersive Fourier transform spectroscopy system (DFTS) are compared and analyzed. Data measured by the frequency variation technique were seen to be more accurate than those measured by the full cavity length variation technique with lower random errors for the specimens measured. The ε' of the specimens measured by the frequency variation technique followed closely with those measured by the millimeter-wave DFTS system with a slight difference of about 0.02%. Finally, for all the specimens measured in this paper, the DFTS system was seen to provide much better accuracy for ε' values. The frequency variation technique from the open resonator system generated the best tanδ.