Microwave dielectric loss tangent measurements are demonstrated as a method for quantifying trace sp-hybridized carbon impurities in sub-micron diamond powders. Appropriate test samples are prepared by vacuum annealing at temperatures from 600 to 1200 °C to vary the sp/sp carbon ratio through partial surface graphitization. Microwave permittivity measurements are compared with those obtained using X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and electron energy loss spectroscopy (EELS). The average particle size remains constant (verified by scanning electron microscopy) to decouple any geometric dielectric effects from the microwave measurements. After annealing, a small increase in sp carbon was identified from the XPS C 1s and Auger spectra, the EELS σ* peak in the C 1s spectra, and the D and G bands in Raman spectroscopy, although a quantifiable diamond to G-band peak ratio was unobtainable. Surface hydrogenation was also evidenced in the Raman and XPS O 1s data. Microwave cavity perturbation measurements show that the dielectric loss tangent increases with increasing sp bonding, with the most pertinent finding being that these values correlate with other measurements and that trace concentrations of sp carbon as small as 5% can be detected.