X-ray, neutron and gamma ray diffraction rocking curves; X-ray topography; microhardness; and optical microscopic measurements have been performed directly on several mercuric iodide (Hgl2) nuclear radiation detectors fabricated from single crystals grown from the vapor phase. Two types of detectors were measured: spectrometer types (grades A and B), which had resolutions of 5–10% for the 662 keV photopeak of 137Cs, or radiation counters (grades C and D), where the spectral resolution ranged from 11% to no resolution. A good correlation has been found between the detector grade and the full width at half maximum (FWHM) of both the X- and gamma ray rocking curves (i.e., the higher the detector grade (A or B), the narrower the FWHM of the diffraction peak). X-ray topography also correlated with well both the FWHM of the diffraction X-ray rocking curve and the detector grade. The uniformity of the microhardness of the HgI2 detectors was found to be proportional to the nuclear performance of the detector. The better spectrometer-grade detectors were softer and much more uniform in microhardness than the most inferior detectors. The better detectors were also found to have much smoother surfaces than the poorer detectors, as observed by optical microscopy studies.