Ferromagnetic insulators with ultra-low damping and tunable magnetic properties are of great interest for the study of spin wave-based phenomena as well as for applications in spin wave spintronics. We have developed epitaxial spinel structure ferrite thin films of Li0.5(AlxFe2.5−x)O4 (LAFO) with ultra-low magnetic damping. The degree of Al substitution tunes the saturation magnetization and in-plane magnetic anisotropy while maintaining excellent epitaxy and crystalline quality as well as low magnetic damping. All LAFO films, deposited on (001)-oriented MgAl2O4 (MAO), are under epitaxial compressive strain, giving rise to an easy magnetic axis in-plane and a hard out-of-plane axis. Element-specific x-ray magnetic circular dichroism measurements confirm that the magnetism originates from the majority of Fe3+ cations occupying the octahedral sites, which are displaced by increased Al3+ substitution. Broadband ferromagnetic resonance reveals the lowest Gilbert damping parameters of 5×10−4 for films 10–15 nm thick. Our films demonstrate the robustness of the low loss dynamic properties of Li0.5(AlxFe2.5−x)O4 that are promising for spin wave applications.