The susceptibility of layered structures to stacking faults is a problem in some of the more attractive semiconductor materials for ambient-temperature radiation detectors. In this work, Bridgman-grown BiI3 layered single crystals are investigated to understand and eliminate structural disorder, which reduces radiation detector performance. The use of superheating gradients has been shown by others to improve crystal quality in non-layered semiconductor crystals (Rudolph et al., 1996) [26]; thus the technique was explored to improve the growth of BiI3. When investigating the homogeneity of non-superheated crystals, highly geometric void defects were found to populate the bulk of the crystals. Applying a superheating gradient to the melt prior to crystal growth improved structural quality and decreased defect density from the order of 4600 voids per cm(3) to 300 voids per cm(3). Corresponding moderate improvements to electronic properties also resulted from the superheat gradient method of crystal growth. Comparative measurements through infrared microscopy, etch-pit density, X-ray rocking curves, and sheet resistivity readings show that superheat gradients in BiI3 growth led to higher quality crystals. (C) 2015 Elsevier B.V. All rights reserved.