Mn+1AXn (MAX) phases are novel structural and functional materials with a layered crystal structure. Their unique properties such as good machinability, high electrical conductivity, low friction, and corrosion resistance are appealing for many engineering applications. Herein, Ti2AlC and Ti3AlC2 MAX thin films are synthesized by magnetron sputtering and subsequent thermal annealing. A multilayer approach is used to deposit single-element nanolayers of titanium, aluminum, and carbon onto silicon substrates with a double-layer-diffusion barrier of SiO2 and SixNy. Ti2AlC and Ti3AlC2 thin films (thickness ≈500 nm) are formed via rapid thermal annealing and verified by X-Ray diffraction. Nanoindentation tests show hardness values of about 11.6 and 5.3 GPa for Ti2AlC and Ti3AlC2, respectively. The tribological behavior of the Ti2AlC and Ti3AlC2 thin films against AISI 52100 steel balls under dry sliding conditions is studied using ball-on-flat tribometry. The resulting coefficient of friction (CoF) for Ti2AlC and Ti3AlC2 ranges between 0.21–0.42 and 0.64–0.91, respectively. The better tribological behavior observed for Ti2AlC thin films is ascribed to its smaller grain size, reduced surface roughness, and higher hardness.