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The objective of this work is to review and assess the potential of MgB4O7:Ce,Li to fill in the gaps where the need for a new material for optically stimulated luminescence (OSL) dosimetry has been identified. We offer a critical assessment of the operational properties of MgB4O7:Ce,Li for OSL dosimetry, as reviewed in the literature and complemented by measurements of thermoluminescence spectroscopy, sensitivity, thermal stability, lifetime of the luminescence emission, dose response at high doses (>1000 Gy), fading and bleachability. Overall, compared with Al2O3:C, for example, MgB4O7:Ce,Li shows a comparable OSL signal intensity following exposure to ionizing radiation, a higher saturation limit (ca 7000 Gy) and a shorter luminescence lifetime (31.5 ns). MgB4O7:Ce,Li is, however, not yet an optimum material for OSL dosimetry, as it exhibits anomalous fading and shallow traps. Further optimization is therefore needed, and possible avenues of investigation encompass gaining a better understanding of the roles of the synthesis route and dopants and of the nature of defects.