Spinels represent a small fraction of lunar surface materials but provide important insights into the petrological evolution of the lunar crust and mantle. Previous remote sensing analyses of highlands spinel‐bearing lithologies have focused on pure Mg‐Al spinels, which are rare in the lunar sample collection. Using Moon Mineralogy Mapper data, we develop and test an approach for detecting spectral signatures of spinel across a wider range of Mg, Al, Fe, Cr, Ti‐bearing compositions than have been addressed in previous studies, including within mafic‐bearing assemblages. This approach is validated through integration with laboratory‐measured spinel spectra and petrographic observations of samples returned by the Luna 20 mission from the Hilly and Furrowed Terrain surrounding the Crisium Basin. Applying this approach to data from the Crisium region, small abundances of spinel (<∼5 vol%) with a range of Mg, Al, Fe, Cr, and Ti content and petrologic origin (inferred from Luna 20 samples) were found to be widespread within highlands soils across the Crisium region. This result diverges from previous remote sensing analyses, which only reported small, isolated exposures of pure Mg‐Al spinel (as well as a possible detection of Fe, Cr‐bearing spinels localized within pyroclastic materials at Sinus Aestuum). Geologic associations of candidate spinel detections across this region are consistent with a shallow crustal origin rather than excavation from depth during the Crisium‐forming impact. These spinels are detectible in near‐infrared spectroscopic data, particularly in areas of low optical maturity and may influence the spectral continuum of highlands soils.