Optically stimulated luminescence (OSL) detectors (OSLDs) have shown potential for measurements of linear energy transfer (LET) in proton therapy beams. However, the technique lacks the efficiency needed for clinical implementation, and a faster, simpler approach to LET measurements is desirable. The goal of this work was to demonstrate and evaluate the potential of calibrating Al2O3:C OSLDs for LET measurements using new methods. We exposed batches of OSLDs to unmodulated proton beams of varying LET and calibrated three parameters of the resulting OSL signals as functions of fluence-averaged LET (ϕ-LET) and dose-averaged LET (D-LET). These three parameters included the OSL curve shape evaluated under continuous wave stimulation (CW-OSL), the OSL curve shape evaluated under pulsed stimulation (P-OSL), and the intensity ratio of the two main emission bands in the Al2O3:C OSL emission spectrum (ultraviolet [UV]/blue ratio). To test the calibration, we then irradiated new batches of OSLDs in modulated proton beams of varying LET, and used the OSL signal parameters to calculate ϕ-LET and D-LET under these new test conditions. Using the P-OSL curve shape, D-LET was measured within 5.7% of the expected value. We conclude that from a single 10 s readout (following initial calibration), both the absorbed dose and LET in proton therapy beams can be measured using OSLDs. This has potential future applications in the quality assurance of proton therapy treatment plans, particularly for those that may account for LET or relative biological effectiveness in their optimization. The methods demonstrated in this work may also be applicable to other particle therapy beams, including carbon ion beams.