Dissolved compounds and ions, including mineral elements and products of microbial metabolism, are present in many cheeses in relatively high concentrations. These dissolved substances may precipitate from the aqueous phase of cheese to form sparingly soluble crystals that can impart a crunchy, gritty, or sandy texture on the cheese. In the present work, optical and diffractometric methods were optimized for use with cheese samples to identify crystal phases in several cheese varieties. These techniques, which included powder X-ray diffractometry (PXRD), single crystal X-ray diffractometry (SCXRD), and petrographic microscopy (PM) have traditionally been used on geological specimens that are quite different from the cheese samples used in the present study. Nonetheless, these techniques were successfully used to gain valuable insight into crystal development in cheese. Powder X-ray diffractometry was optimized to minimize the occurrence of artifacts that may occur due to the high water content and low crystallinity of some cheese samples. The use of enhanced sample preparation techniques facilitated the identification of organic and inorganic crystal phases such as tyrosine, leucine, brushite (CaHPO4·2H2O), and calcite (CaCO3) in hard and soft cheeses. SCXRD was used to determine the crystal structures of ikaite and struvite, which had been tentatively identified in washed-rind cheese using PXRD. PM was used to observe morphological and optical properties of crystals in white mold cheese and washed-rind cheese. In two subsequent aging studies, PXRD was used to determine the approximate timing of crystal nucleation in the rinds of white mold cheese and washed-rind cheese. These observations were paired with inductively coupled plasma-atomic emission spectroscopy (ICP-AES) data to demonstrate that the onset of crystallization in the rinds coincided with a diffusion phenomenon in which mineral ions diffused from the center of the cheese and became concentrated in the rind. PM observations demonstrated that maximum crystal size in the rinds generally increased as aging progressed. These observations will be useful in future work that investigates the impact of crystallization on sensory properties of cheese.