A magnetic atom in a superconducting host induces so-called Yu-Shiba-Rusinov (YSR) bound states inside the superconducting energy gap. By combining spin-resolved scanning tunneling spectroscopy with simulations we demonstrate that the pair of peaks associated with the YSR states of an individual Fe atom coupled to an oxygen-reconstructed Ta surface gets spin polarized in an external magnetic field. As theoretically predicted, the electron and hole parts of the YSR states have opposite signs of spin polarizations which keep their spin character when crossing the Fermi level through the quantum phase transition. The simulation of a YSR state right at the Fermi level reveals zero spin polarization which can be used to distinguish such states from Majorana zero modes in chains of YSR atoms. DOI: 10.1103/PhysRevLett.119.197002 Recent investigations of chains [1][2][3] and arrays [4,5] of magnetic atoms in contact with surfaces of s-wave superconductors in view of Majorana zero modes and topological superconductivity triggered renewed interest in the properties of the basic constituent of such systems, the individual magnetic adatom. Typically, such adatoms induce quasiparticle excitations inside the superconducting energy gap [6][7][8], referred to as Yu-Shiba-Rusinov (YSR) states, which hamper the identification of topologically nontrivial edge states [3,9], calling for a thorough characterization of all experimentally accessible properties of YSR states.Following the first experimental verification of YSR states of individual atoms using scanning tunneling spectroscopy (STS) [10], there were numerous experimental studies, focusing on orbital effects [11][12][13], magnetic anisotropy [14], effects of reduced dimensionality of the superconductor [15], effects of coupling [11,16], and the competition between Kondo screening and superconducting pairing [17,18]. However, the investigation of the spin polarization of the YSR state of individual atoms, which could serve as a fingerprint for the distinction from topological states [19], was so far restricted to theoretical predictions [6][7][8][20][21][22].Neglecting orbital effects or magnetic anisotropy, theory predicts one pair of spin-polarized states of a YSR atom, an electron (e − )-and a hole (h)-like part with opposite spin character, which are located at AEjεj from the Fermi level E F [20]. There is a pronounced asymmetry in spectral weight between the e − and h parts due to electron-hole asymmetry of the band structure [21,22] and/or a nonmagnetic scattering potential of the impurity [20,23]. With increasing exchange coupling J between the adatom and substrate, the binding energy ε decreases until the YSR states eventually cross E F through a quantum phase transition (QPT), accompanied by an inversion of the asymmetry in the e − − h spectral weight [17]. Most notably, since both parts of the YSR states keep their spin character, the spin polarization above and below E F is expected to invert [20] through the QPT. Here, we experimentally verify these prediction...