With a growing demand for the rare earth elements (REE), exploration of regolith-hosted REE resources worldwide has been thriving in recent years and development of a rapid and reliable field-based tool will greatly facilitate the survey and exploration. In this study, we use visible and short-wave infrared (VNIR-SWIR) reflectance spectroscopy to comprehensively evaluate the applicability of the technique to explore regolith-hosted REE resources, exemplified by three representative regolith-hosted REE deposits in China. Neodymium among the REE shows reliably detectable spectral features in the VNIR-SWIR spectroscopy down to concentrations of 10–50 ppm in field samples with heterogeneous mineral grain sizes. The Nd spectral intensity of electronic transition at the band of ∼800 nm is correlated with bulk Nd concentrations and can be used as semi-quantitative indicators for the Nd concentrations, thereby the total REE in regolith. Moreover, VNIR-SWIR spectroscopy is demonstrated to be capable of delineating favorable ore-bearing mineralogy by characterizing the abundance and type of clay minerals and Fe (oxyhydr)oxides, and the crystallinity of kaolinite-group minerals. However, the Nd spectral features of samples with high bulk Fe₂O₃ contents (>3 wt%) are significantly masked due to overlapping by the strong absorption features of ferric (oxyhydr)oxides. VNIR-SWIR spectroscopy is deemed to be applicable to the exploration of regolith-hosted REE resources developed from Fe-poor felsic rocks.