AbstractPhotochromic sodalites are considered for a plethora of possible applications, such as UV indexing and X‐ray imaging, but for many of these the materials are yet to be optimized. UV indexing can be improved through incremental adjustment of the activation energy of coloration from 300 to 410 nm through replacement of sulfur with selenium. By combining this and other methods of tuning presented in the literature, the excitation threshold and photochromism color can be tuned independently of one another. The range of possible absorption maxima is expanded to 420–680 nm, or almost the entire visible spectrum. Mixing low‐cost and easy‐to‐synthesize sodalites further broadens the possible range of colors and facilitates development of a unique sodalite mix capable of quantifying the doses of two types of UV radiation simultaneously. Finally, the response to X‐rays of these highly tuned sodalites is investigated, and it is found that they can be sensitized to produce clear, high‐contrast X‐ray images at significantly lower doses of radiation than those required by classic photochromic sodalite, Na8(AlSiO4)6(Cl,S)2.