The quest for new materials for thermoluminescence (TL) and optically stimulated luminescence (OSL) dosimetry continues to be a central line of research in luminescence dosimetry, occupying many groups and investigators, and is the topic of many publications. Nevertheless, it has also been a research area with many pitfalls, slow advances in our understanding of the luminescence processes, and rare improvements over existing materials. Therefore, this paper reviews the status of the field with the goal of addressing some fundamental questions: Is there a need for new luminescence materials for TL/OSL dosimetry? Can these materials be designed and, if so, are there strategies or rules that can be followed? What are the common pitfalls and how can they be avoided? By discussing these questions, we hope to contribute to a more guided approach to the development of new luminescent materials for dosimetry applications.