In this study, different interpolation techniques are presented, assessed, and compared for the estimation of soil iron (Fe) contents in locations where observations were not available. Initially, 400 soil samples from the Kozani area, which is near Polifitou Lake in northern Greece, were randomly collected from 2013 to 2015 and were analysed in the laboratory to determine the soil Fe concentrations and pH. The soil Fe concentrations were examined for spatial autocorrelation, and semivariograms were used to determine whether pH and Fe exhibited spatial cross correlation. Three interpolation methods, including Ordinary Kriging, Universal Kriging, and Co-Kriging, were applied, and their results were compared with the use of two different cross-validation methods. In the current study, there was evidence of spatial cross correlation of soil Fe and pH for each year, which was subsequently used to improve the interpolation results in locations where there were no measurements. In nearly all cases, Co-Kriging, which takes advantage of the covariance between the two regionalized variables (Fe and pH), outperformed the other interpolation techniques each year.