To address the global phenomenon of the salinisation of large land areas, a quantitative inversion model of the salinity of saline soils and soil visible–near-infrared (NIR) spectral data was developed by considering saline soils in Zhenlai County, Jilin Province, China as the research object. The original spectral data were first subjected to Savitzky–Golay (SG) smoothing, multiplicative scattering correction (MSC) pre-processing, and a combined transformation technique. The pre-processed spectral data were then analysed to construct the difference index (DI), ratio index (RI), and normalised difference index (NDI), and the Spearman rank correlation coefficient (r) between these three spectral indices and the salt content in the samples was calculated, while a combined spectral index (r > 0.8) was eventually selected as a sensitive spectral index. Finally, a quantitative inversion model for the salinity of saline soils was developed, and the model’s accuracy was evaluated based on partial least squares regression (PLSR), the random forest (RF) algorithm, and the radial basis function (RBF) neural network algorithm. The results indicated that the inversion of soil salt content using the selected combination of spectral indices based on the RBF neural network algorithm was the most effective, with the prediction model yielding an R² value of 0.950, a root mean square error (RMSE) of 1.014, and a relative percentage deviation (RPD) of 4.479, which suggested a good prediction effect.