Tuning the magnetic properties of materials is a demand of several technologies; however, our microscopic understanding of the process that drives the enhancement of those properties is still unsatisfactory. In this work, we combined experimental and theoretical techniques to investigate the handling of magnetic properties of FeCo thin films via the thickness-tuning of a gold film used as an underlayer. We grow the samples by the deposition of polycrystalline FeCo thin films on the Au underlayer at room temperature by a magnetron sputtering technique, demonstrating that the lattice parameter of the sub-20 nm thickness gold underlayer is dependent on its thickness, inducing a stress up to 3% in sub-5 nm FeCo thin films deposited over it. Thus, elastic-driven variations for the in-plane magnetic anisotropy energy, K u , up to 110% are found from our experiments. Our experimental findings are in excellent agreement with ab initio quantum chemistry calculations based on density functional theory, which helps to build up an atomistic understanding of the effects that take place in the tuning of the magnetic properties addressed in this work. The handling mechanism reported here should be applied to other magnetic films deposited on different metallic underlayers, opening possibilities for large-scale fabrication of magnetic components to be used in future devices.