The spatial distribution of precipitation is one of the most important climatic variables used in geographic and environmental studies. However, when there is a lack of full coverage of meteorological stations, precipitation estimations are necessary to interpolate precipitation for larger areas. The purpose of this research was to find the best interpolation method for precipitation mapping in the partly densely populated Khorasan Razavi province of northeastern Iran. To achieve this, we compared five methods by applying average precipitation data from 97 rain gauge stations in that province for a period of 20 years (1994–2014): Inverse Distance Weighting, Radial Basis Functions (Completely Regularized Spline, Spline with Tension, Multiquadric, Inverse Multiquadric, Thin Plate Spline), Kriging (Simple, Ordinary, Universal), Co-Kriging (Simple, Ordinary, Universal) with an auxiliary elevation parameter, and non-linear Regression. Root Mean Square Error (RMSE), Mean Absolute Error (MAE), and the Coefficient of Determination (R2) were used to determine the best-performing method of precipitation interpolation. Our study shows that Ordinary Co-Kriging with an auxiliary elevation parameter was the best method for determining the distribution of annual precipitation for this region, showing the highest coefficient of determination of 0.46% between estimated and observed values. Therefore, the application of this method of precipitation mapping would form a mandatory base for regional planning and policy making in the arid to semi-arid Khorasan Razavi province during the future.