Laser surface texturing is an efficient way to control the friction and wear properties of materials. Although described in many papers, most previous work relates to a pure topographic view of laser-textured surfaces. As lasers are heat sources, their thermal impact during treatment can be high enough to modify the material’s microstructure or surface chemistry and affect tribological properties as well. This research took a closer look at the microstructure of laser-textured TiAl multilayers, besides topographic aspects. Direct laser interference patterning was used to create well-defined line-like surface textures in TiAl multilayers with differing lateral feature sizes in the micron range. High-resolution techniques such as TEM and XRD highlighted the effect of this method on microstructure, and in particular, the phase situation of the TiAl multilayer. Thermal simulations demonstrated that the maximum achievable temperatures were around 2000 K, thus being high enough to melt Ti and Al. Cooling rates on the order of 109 K/s depended on the lateral feature size, potentially leading to metastable microstructures. Finally, ball-on-disk tests on as-textured TiAl specimens showed a reduction in wear under dry conditions depending on the periodicity of the line-like textures used.