Spintronics exploits the magnetoresistance effects to store or sense the magnetic information. Since the magnetoresistance strictly depends on the magnetic anisotropy of the system, it is fundamental to set a defined anisotropy to the system. Here, we investigate by means of vectorial Magneto-Optical Kerr Magnetometry (v-MOKE), half-metallic La0.67Sr0.33MnO3 (LSMO) thin films that exhibit at room temperature pure biaxial magnetic anisotropy if grown onto MgO (001) substrate with a thin SrTiO3 (STO) buffer. In this way, we can avoid unwanted uniaxial magnetic anisotropy contributions that may be detrimental for specific applications. The detailed study of the angular evolution of the magnetization reversal pathways, critical fields (coercivity and switching) allows for disclosing the origin of the magnetic anisotropy, which is magnetocrystalline in nature and shows four-fold symmetry at any temperature.Half-metallic perovskite oxides promise great advantages over conventional spintronics metallic materials for applications such as magnetic sensors, magnetic random access memory (MRAM), magnetic tunnel junctions (MTJs) and domain wall race-track memories. 1 Perovskite oxides, in general, appear to be a new contender for many novel applications that were considered traditionally beyond its range. 2 The conduction mechanism in these materials, in fact, strongly depends on the interplay between orbital and spin degrees of freedom 3 that may be exploited to add multiferroic or ferroelectric functionalities. [4][5][6] The complexity of such mechanism, however, can determine entangled magneto transport response becoming in some cases undesired. For example, it has been seen that a switchable anisotropic magnetoresistance (AMR) response in manganites may be hidden by the colossal magnetoresistance (CMR) if the magnetic anisotropy of the system is not accurately designed. 7 Irrespective of the applications, one of a)