These files contain data supporting all results reported in Pal et al., "Low-temperature spin dynamics in LAFO thin films: from cubic anisotropy to TLS-limited coherence." In this work we investigate the low-temperature spin dynamics of epitaxial lithium aluminum ferrite (LAFO) thin films using broadband ferromagnetic resonance (FMR) spectroscopy from 0.44 K to 68 K. The results reveal a crossover from conventional cubic anisotropy-dominated behavior at higher temperatures to pronounced linewidth broadening and higher-order anisotropy contributions at cryogenic temperatures. With the magnetic field oriented along the [100] crystallographic direction, the resonance is well-captured by four-fold in-plane and out-of-plane uniaxial anisotropies. In contrast, measurements with the field along the [110] direction reveal the presence of an unusually large sixth-order cubic anisotropy term that is symmetry-suppressed for [100] but becomes apparent under this field orientation at ultralow temperatures, indicating a substantial modification of the anisotropy landscape. Independent linewidth analysis shows a pronounced peak near 8 K and a subtle monotonic enhancement with decreasing temperatures below 2 K, features consistent with dissipation mediated by a bath of two-level systems (TLS) arising from antisite defects and localized Fe$^{3+}$ moments. Comparison with TLS-based models demonstrates that both exchange-coupled impurities and nearly free paramagnetic centers contribute to the observed damping. Our results establish LAFO as a model ferrite system where disorder-induced TLS limit spin coherence at ultralow temperatures, providing new insights into anisotropy engineering, magnetic relaxation, and the design of ferrimagnetic insulators for coherent magnonics. These findings offer a framework for future optimization of growth conditions.