Cratylia argentea is a leguminous shrub that has the potential for use as livestock feed in tropical areas. However, time-consuming and labor-intensive methods of chemical analysis limit the understanding of its nutritive value. Near-infrared spectroscopy (NIRS) is a low-cost technology widely used in forage crops to expedite chemical composition assessment. The objective of this study was to develop prediction models to assess the crude protein (CP), neutral detergent fiber (NDF), acid detergent fiber (ADF), and dry matter (DM) of Cratylia based on NIRS and partial least squares analysis. A total of 155 samples were harvested at different maturity levels and used for model development, of which 107 were used for calibration and 48 for external validation. The cross-validation presented a root mean square error of prediction of 0.77, 2.56, 3.43, and 0.42; a ratio of performance to deviation of 4.8, 4.0, 3.8, and 3.4; and an R2 of 0.92, 0.92, 0.87, and 0.84 for CP, NDF, ADF, and DM, respectively. Based on the obtained results, we concluded that NIRS accurately predicted the chemical parameters of Cratylia. Therefore, NIRS can serve as a useful tool for livestock producers and researchers to estimate Cratylia’s nutritive value.