Milk and dairy products are a major source of minerals, particularly calcium, involved in several metabolic functions in humans. Currently, several dairy products are enriched with calcium to prevent osteoporosis. The development of an inexpensive and fast quantitative analysis for minerals is required to offer dairy farmers an opportunity to improve the added value of the produced milk. The aim of this study was to develop 5 equations to measure Ca, K, Mg, Na, and P contents directly in bovine milk using mid-infrared (MIR) spectrometry. A total of 1,543 milk samples were collected between March 2005 and May 2006 from 478 cows during the Walloon milk recording and analyzed by MIR spectrometry. Using a principal component approach, 62 milk samples were selected by their spectral variability and separated in 2 calibration sets. Five outliers were detected and deleted. The mineral contents of the selected samples were measured by inductively coupled plasma atomic emission spectrometry. Using partial least squares combined with a repeatability file, 5 calibration equations were built to estimate the contents of Ca, K, Mg, Na, and P in milk. To assess the accuracy of the developed equations, a full cross-validation and an external validation were performed. The cross-validation coefficients of determination (R(2)cv) were 0.80, 0.70, and 0.79 for Ca, Na, and P, respectively (n = 57), and 0.23 and 0.50 for K and Mg, respectively (n = 31). Only Ca, Na, and P equations showed sufficient R(2)cv for a potential application. These equations were validated using 30 new milk samples. The validation coefficients of determination were 0.97, 0.14, and 0.88 for Ca, Na, and P, respectively, suggesting the potential to use the Ca and P calibration equations. The last 30 samples were added to the initial milk samples and the calibration equations were rebuilt. The R(2)cv for Ca, K, Mg, Na, and P were 0.87, 0.36, 0.65, 0.65, and 0.85, respectively, confirming the potential utilization of the Ca and P equations. Even if new samples should be added in the calibration set, the first results of this study showed the feasibility to quantify the calcium and phosphorus directly in bovine milk using MIR spectrometry.