Graphene vertical bar metal vertical bar ligand systems open a new realm in surface magnetochemistry. We show that by trapping metal atoms In the two-dimensional potential lattice of a graphene-ligand interface it is possible to build a chemical analogue of an optical lattice, a key setup in quantum information and strongly correlated systems. Employing sophisticated first-principles calculations, we studied electronic and dynamic properties of graphene vertical bar metal vertical bar ligand assemblies and showed that there is a general principle-spin-charge separation in pi-d systems-that underlies the possibility of synthesizing and controlling such systems. We find that ligands can work as a local gate to control the properties of trapped metal atoms and can impose bosonic or fermionic character on such atomic nets, depending on the ligand's nature. Remarkably, the magnetization energy in such systems reaches record-high values of ca. 400 meV, which makes the respective magnetic phenomena utilizable at room temperature. Accompanied by spin polarization of the graphene pi-conjugated system it leads to spin-valve materials and brings the realization of quantum computing one step closer.