The use of hyperspectral data to estimate forage nutrient content can be a challenging task, considering the multicollinearity problem, which is often caused by high data dimensionality. We predicted some variability in the concentration of limiting nutrients such as nitrogen (N), crude protein (CP), moisture, and non-digestible fibres that constrain the intake rate of herbivores. In situ hyperspectral reflectance measurements were performed at full canopy cover for C3 and C4 grass species in a montane grassland environment. The recorded spectra were resampled to 13 selected band centres of known absorption and/or reflectance features, WorldView-2 band settings, and to 10 nm-wide bandwidths across the 400–2500 nm optical region. The predictive accuracy of the resultant wavebands was assessed using partial least squares regression (PLSR) and an accompanying variable importance (VIP) projection. The results indicated that prediction accuracies ranging from 66% to 32% of the variance in N, CP, moisture, and fibre concentrations can be achieved using the spectral-only information. The red, red-edge, and shortwave infrared (SWIR) wavelength regions were the most sensitive to all nutrient variables, with higher VIP values. Moreover, the PLSR model constructed based on spectra resampled around the 13 preselected band centres yielded the highest sensitivity to the predicted nutrient variables. The results of this study thus suggest that the use of the spectral resampling technique that uses only a few but strategically selected band centres of known absorption or reflectance features is sufficient for forage nutrient estimation.