Mid-infrared (MIR) spectroscopy is emerging as one of the most promising technologies, as it is a rapid and cost-effective alternative to routine laboratory analysis for many soil properties. This study was conducted to evaluate the potential of mid-infrared spectroscopy for the rapid and nondestructive measurement of some important soil properties of Alfisols. A total of 336 georeferenced soil samples fromthe 0–15 cm soil layer of Alfisols that were collected from the eastern Indian states of Odisha and Jharkhand were used. The partial least-squares regression (PLSR), random forest, and support vector machine regression techniques were compared for the calibration of the spectral data with the wet chemistry soil data. The PLSR-based predictive models performed better than the other two regression techniques for all the soil properties, except for the electrical conductivity (EC). Good predictions with independent validation datasets were obtained for the clay and sand percentages and for the soil organic carbon (SOC) content, while satisfactory predictions were achieved for the silt percentage and the pH value. However, the performance of the predictive models was poor in the case of the EC and the extractable nutrients, such as the available phosphorus and potassium contents of the soil. Specific regions of the MIR spectra that contributed to the prediction of the soil SOC, the pH, and the clay and sand percentages were identified. The study demonstrates the potential of the MIR spectroscopic technique in the simultaneous estimation of the SOC content, the sand, clay, and silt percentages, and the pH of Alfisols from eastern India.