Soil salinization is one of the most common land degradation processes and is a severe environmental hazard. The primary objective of this study is to investigate the potential of predicting salt content in soils with hyperspectral data acquired with EO-1 Hyperion. Both partial least-squares regression (PLSR) and conventional multiple linear regression (MLR), such as stepwise regression (SWR), were tested as the prediction model. PLSR is commonly used to overcome the problem caused by high-dimensional and correlated predictors. Chemical analysis of 95 samples collected from the top layer of soils in the Yellow River delta area shows that salt content was high on average, and the dominant chemicals in the saline soil were NaCl and MgCl₂. Multivariate models were established between soil contents and hyperspectral data. Our results indicate that the PLSR technique with laboratory spectral data has a strong prediction capacity. Spectral bands at 1487–1527, 1971–1991, 2032–2092, and 2163–2355 nm possessed large absolute values of regression coefficients, with the largest coefficient at 2203 nm. We obtained a root mean squared error (RMSE) for calibration (with 61 samples) of RMSE_C = 0.753 (R² = 0.893) and a root mean squared error for validation (with 30 samples) of RMSE_V = 0.574. The prediction model was applied on a pixel-by-pixel basis to a Hyperion reflectance image to yield a quantitative surface distribution map of soil salt content. The result was validated successfully from 38 sampling points. We obtained an RMSE estimate of 1.037 (R² = 0.784) for the soil salt content map derived by the PLSR model. The salinity map derived from the SWR model shows that the predicted value is higher than the true value. These results demonstrate that the PLSR method is a more suitable technique than stepwise regression for quantitative estimation of soil salt content in a large area.