Ge_1−xSn_x and Si_1−x−yGe_ySn_x alloys are promising materials for future opto- and nanoelectronics applications. These alloys enable effective bandgap engineering, broad adjustability of their lattice parameter, exhibit much higher carrier mobility than pure Si, and are compatible with the complementary metal-oxide-semiconductor technology. Unfortunately, the equilibrium solid solubility of Sn in Si_1−xGe_x is less than 1% and the pseudomorphic growth of Si_1−x−yGe_ySn_x on Ge or Si can cause in-plane compressive strain in the grown layer, degrading the superior properties of these alloys. Therefore, post-growth strain engineering by ultrafast non-equilibrium thermal treatments like pulse laser annealing (PLA) is needed to improve the layer quality. In this article, Ge_0.94Sn_0.06 and Si_0.14Ge_0.8Sn_0.06 thin films grown on silicon-on-insulator substrates by molecular beam epitaxy were post-growth thermally treated by PLA. The material is analyzed before and after the thermal treatments by transmission electron microscopy, x-ray diffraction (XRD), Rutherford backscattering spectrometry, secondary ion mass spectrometry, and Hall-effect measurements. It is shown that after annealing, the material is single-crystalline with improved crystallinity than the as-grown layer.