This work elucidates the effect of the dopant aluminum on the growth of magnetron-sputtered aluminum-doped zinc oxide (ZnO:Al) films by means of a seed layer concept. Thin (<100 nm), highly doped seed layers and subsequently grown thick (∼800 nm), lowly doped bulk films were deposited using a ZnO:Al2O3 target with 2 wt. % and 1 wt. % Al2O3, respectively. We investigated the effect of bulk and seed layer deposition temperature as well as seed layer thickness on electrical, optical, and structural properties of ZnO:Al films. A reduction of deposition temperature by 100 °C was achieved without deteriorating conductivity, transparency, and etching morphology which renders these low-temperature films applicable as light-scattering front contact for thin-film silicon solar cells. Lowly doped bulk layers on highly doped seed layers showed smaller grains and lower surface roughness than their counterpart without seed layer. We attributed this observation to the beneficial role of the dopant aluminum that induces an enhanced surface diffusion length via a surfactant effect. The enhanced surface diffusion length promotes 2D-growth of the highly doped seed layer, which is then adopted by the subsequently grown and lowly doped bulk layer. Furthermore, we explained the seed layer induced increase of tensile stress on the basis of the grain boundary relaxation model. The model relates the grain size reduction to the tensile stress increase within the ZnO:Al films. Finally, temperature-dependent conductivity measurements, optical fits, and etching characteristics revealed that seed layers reduced grain boundary scattering. Thus, seed layers induced optimized grain boundary morphology with the result of a higher charge carrier mobility and more suitable etching characteristics. It is particularly compelling that we observed smaller grains to correlate with an enhanced charge carrier mobility. A seed layer thickness of 5 nm was sufficient to induce the beneficial effects.