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The material family halide perovskites has been critical in recent room-temperature radiation detection semiconductor research. Cesium lead bromide (CsPbBr3) is a halide perovskite that exhibits characteristics of a semiconductor that would be suitable for applications in various fields. In this paper, we report on the correlations between material purification and crystal material properties. Crystal boules of CsPbX3 (where X = Cl, Br, I, or mixed) were grown with the Bridgman growth method. We describe in great detail the fabrication techniques used to prepare sample surfaces for contact deposition and sample testing. Current–voltage measurements, UV–Vis and photocurrent spectroscopy, as well as photoluminescence measurements, were carried out for material characterization. Bulk resistivity values of up to 3.0 × 109 Ω∙cm and surface resistivity values of 1.3 × 1011 Ω/□ indicate that the material can be used for low-noise semiconductor detector applications. Preliminary radiation detectors were fabricated, and using photocurrent measurements we have estimated a value of the mobility–lifetime product for holes (μτ)h of 2.8 × 10−5 cm2/V. The results from the sample testing can shed light on ways to improve the crystal properties for future work, not only for CsPbX3 but also other halide perovskites.