Lithium titanate (Li4Ti5O12) is a commercial anode material used for high-power and long-lifespan lithium batteries. The key drawback of this material is its low electronic conductivity. Although doping is commonly used to solve this problem, the introduction of dopants also diminished lattice stability. In this work, we studied fast and slow laser-induced degradation processes of single Mn-doped lithium titanate particles and proposed a physicochemical model of their degradation mechanism. We suppose that the preferable route of LTO alteration is the formation of amorphous phases rather than crystalline decomposition products. Our results may be useful for not only developing a nondestructive characterization tool utilizing Raman spectroscopy but also for understanding other degradation processes, including thermal alteration and structural changes caused by the intercalation/deintercalation cycles of lithium ions. © 2022 by the authors.