The laser ablation and deposition of FeSiGaRu is studied. The deposited thin films are analyzed with Auger electron spectroscopy and Rutherford backscattering spectrometry. It is found that the gallium and ruthenium content of the thin films is strongly dependent on the laser fluence. At high laser fluences (6 J/cm2) the thin films are depleted of gallium due to preferential sputtering of the gallium atoms from the thin film. Near the threshold fluence (1.9 J/cm2) the films contain an excess of gallium due to preferential evaporation of gallium from the target. The latter conclusions are based on time‐of‐flight studies of ablated atoms and ions and on measurements of the atoms that are sputtered from the substrate by the incoming flux.