This study explores the use of leaf-level visible-to-shortwave infrared (VSWIR) reflectance observations and partial least squares regression (PLSR) to predict foliar concentrations of macronutrients (nitrogen, phosphorus, potassium, calcium, magnesium, and sulfur), micronutrients (boron, copper, iron, manganese, zinc, molybdenum, aluminum, and sodium), and moisture content in winter wheat. A total of 360 fresh wheat leaf samples were collected from a wheat breeding population over two growing seasons. These leaf samples were used to collect VSWIR reflectance observations across a spectral range spanning 350 to 2,500 nm. These samples were then processed for nutrient composition to allow for the examination of the ability of reflectance to accurately model diverse chemical components in wheat foliage. Models for each nutrient were developed using a rigorous cross-validation methodology in conjunction with three distinct component selection methods to explore the trade-offs between model complexity and performance in the final models. We examined absolute minimum predicted residual error sum of squares (PRESS), backward iteration over PRESS, and Van der Voet’s randomized t-test as component selection methods. In addition to contrasting component selection methods for each leaf trait, the importance of spectral regions through variable importance in projection scores was also examined. In general, the backward iteration method provided strong model performance while reducing model complexity relative to the other selection methods, yielding R2 [relative percent difference (RPD), root mean squared error (RMSE)] values in the validation dataset of 0.84 (2.45, 6.91), 0.75 (1.97, 18.67), 0.78 (2.13, 16.49), 0.66 (1.71, 17.13), 0.68 (1.75, 14.51), 0.66 (1.72, 12.29), and 0.84 (2.46, 2.20) for nitrogen, calcium, magnesium, sulfur, iron, zinc, and moisture content on a wet basis, respectively. These model results demonstrate that VSWIR reflectance in combination with modern statistical modeling techniques provides a powerful high throughput method for the quantification of a wide range of foliar nutrient contents in wheat crops. This work has the potential to advance rapid, precise, and nondestructive field assessments of nutrient contents and deficiencies for precision agricultural management and to advance breeding program assessments.