Manganese, showing stable oxidation states spanning from+ 2 to+ 7, gives rise to a variety of oxides (Mn O x) whose exploitation in several technological fields, such as energy conversion and storage, catalysis, sensing, and environmental and biomedical engineering, is highly promising. Nevertheless, the chemical complexity and the structural richness of Mn O x—involving mixed-valence and metastable species—make the correct identification by Raman spectroscopy challenging, further complicated by the laser sensitivity, poor Raman activity, and conflicting literature scenario. Moreover, a careful optimization of the material in terms of phase, structure, and morphology is highly desirable in view of the final application, where precise control over the materials properties is essential. In this paper, we discuss the capability of room-temperature pulsed laser deposition (PLD) followed by postdeposition thermal …