Clay minerals are the most reactive and important inorganic components in soils, but soil mineralogy classifies as a minor topic in soil sciences. Revisiting soil mineralogy has been gradually required. Clay minerals in soils are more complex and less well crystallized than those in sedimentary rocks, and thus, they display more complicated X-ray diffraction (XRD) patterns. Traditional characterization methods such as XRD are usually expensive and time-consuming, and they are therefore inappropriate for large datasets, whereas visible and near-infrared reflectance spectroscopy (VNIR) is a quick, cost-efficient, and nondestructive technique for analyzing soil mineralogic properties of large datasets. The main objectives of this review are to bring readers up to date with information and understanding of VNIR as it relates to soil mineralogy and attracts more attention from a wide variety of readers to revisit soil mineralogy. We begin our review with a description of fundamentals of VNIR. We then review common methods to process soil VNIR spectra and summary spectral features of soil minerals with particular attention to those <2 μm fractions. We further critically review applications of chemometric methods and related model building in spectroscopic soil mineral studies. We then compare spectral measurement with multivariate calibration methods, and we suggest that they both produce excellent results depending on the situation. Finally, we suggest a few avenues of future research, including the development of theoretical calibrations of VNIR more suitable for various soil samples worldwide, better elucidation of clay mineral-soil organic carbon (SOC) interactions, and building the concept of integrated soil mapping through combined information (e.g., mineral composition, soil organic matter-SOM, SOC, pH, and moisture).