new class of vdW magnets provides the long-sought-after experimental testbeds of the fundamental Hamiltonians of 2D magnetism: Ising, XY, and Heisenberg models. [6] The first experimental test of the Onsager solution of the Ising model was performed on antiferromagnetic FePS 3 , [7] followed by the discovery of 2D ferromagnetic van der Waals materials such as CrGeTe 3 [8] and CrI 3 . [9] Eventually, the XY and Heisenberg models were subsequently realized using NiPS 3 , [10,11] CrCl 3 , [12] and MnPS 3 , [13][14][15] respectively.The investigation of vdW materials has so far focused on 2D magnetic order phenomena, and much less attention has been paid to their microscopic origin. Typically, the role of orbital magnetism is often neglected since the magnetic orbital moment is supposedly quenched in most 3d transition metal based magnetic materials via so-called crystal field splittings due to the interaction with the surrounding atoms. However, systems with reduced symmetry can, in principle, host sizeable magnetic orbital moments approaching those of the respective free atoms. [16,17] In such a case, the spin-orbit interaction can give rise to new phenomena such as spin-orbit entanglement, a manifestation of direct quantum effects in the condensed matter state. [18] Moreover, FePS 3 is-as we will show-a material whose properties are dominated by strong electron correlations. In spinorbit entangled systems, electron spins and orbital motions Van der Waals (vdW) magnets are an ideal platform for tailoring 2D magnetism with immense potential for spintronics applications and are intensively investigated. However, little is known about the microscopic origin of magnetic order in these antiferromagnetic systems. X-ray photoemission electron microscopy is used to address the electronic and magnetic properties of the vdW antiferromagnet FePS 3 down to the monolayer. The experiments reveal a giant out-of-plane magnetic anisotropy of 22 meV per Fe ion, accompanied by unquenched magnetic orbital moments. Moreover, the calculations suggest that the Ising magnetism in FePS 3 is a visible manifestation of spin-orbit entanglement of the Fe 3d electron system.