Visible-near infrared (Vis-NIR) and mid-infrared (MIR) spectroscopy are increasingly being used for the fast determination of soil properties. The aim of this study was (i) to test the use of MIR spectra (Agilent 4300 FTIR Handheld spectrometer) for the prediction of soil properties and (ii) to compare the prediction performances of MIR spectra and Vis-NIR (ASD FieldSpecPro) spectra; the Vis-NIR data were adopted from a previous study. Both the MIR and Vis-NIR spectra were coupled with partial least squares regression, different pre-processing techniques, and the same 114 soil samples, collected from the agricultural land located between boreal forests and semi-arid steppe belts (Kastanozems). The prediction accuracy (R2 = 0.70–0.99) of both techniques was similar for most of the soil properties assessed. However, (i) the MIR spectra were superior for estimating CaCO3, pH, SOC, sand, Ca, Mg, Cd, Fe, Mn, and Pb. (ii) The Vis-NIR spectra provided better results for silt, clay, and K, and (iii) the hygroscopic water content, Cu, P, and Zn were poorly predicted by both methods. The importance of the applied pre-processing techniques was evident, and among others, the first derivative spectra produced more reliable predictions for 11 of the 17 soil properties analyzed. The spectrally active CaCO3 had a dominant contribution in the MIR predictions of spectrally inactive soil properties, followed by SOC and Fe, whereas particle sizes and hygroscopic water content appeared as confounding factors. The estimation of spectrally inactive soil properties was carried out by considering their secondary correlation with carbonates, clay minerals, and organic matter. The soil information covered by the MIR spectra was more meaningful than that covered by the Vis-NIR spectra, while both displayed similar capturing mechanisms. Both the MIR and Vis-NIR spectra seized the same soil information, which may appear as a limiting factor for combining both spectral ranges. The interpretation of MIR spectra allowed us to differentiate non-carbonated and carbonated samples corresponding to carbonate leaching and accumulation zones associated with topography and land use. The prediction capability of the MIR spectra and the content of nutrient elements was highly related to soil-forming factors in the study area, which highlights the importance of local (site-specific) prediction models.