Accurate and rapid determination of moisture content in waste sludge is essential for optimizing dewatering processes, reducing disposal costs, and minimizing environmental impact. This study investigates the use of Fourier Transform Near-Infrared (FT-NIR) spectroscopy combined with Partial Least Squares Regression (PLS-R) for predicting the moisture content of dewatered sludge. A total of 96 sludge samples, with dry matter contents ranging from 12.4% to 24.6%, were collected from two treatment plants. FT-NIR spectra were acquired over the 800–2500 nm range, and chemometric models were developed to correlate spectral information with gravimetrically determined moisture content. The optimized PLS-R model demonstrated strong predictive performance, achieving a cross-validated coefficient of determination (R²CV) of 0.87, a root mean square error of cross-validation (RMSECV) of 0.92%, and a residual predictive deviation (RPD) of 2.73. Independent test set validation confirmed the robustness of the model (R²test = 0.88, RMSEP = 0.88%, RPD = 2.92), supported by strong calibration results (R² = 0.95, RMSEE = 0.60%, RPD = 4.46). Principal component analysis indicated that spectral variability observed in sludge samples was primarily associated with WWTP-specific characteristics, reflecting moisture–organic matter interactions. These results demonstrate that FT-NIR spectroscopy is a promising tool for sludge moisture prediction.