Dimensional confinement of HP lattices via surface coordination of large molecular spacers allows for the formation of distinctive 2D HP structures with various unit thicknesses of inorganic octahedra sheets (described as n), called quasi-2D HPs. The quasi-2D HPs offer more thermodynamically feasible synthesizability, enabling crystallization at relatively lower temperatures while not compromising the overall bandgap of the materials system with respect to 3D counterparts . Furthermore, the molecular spacers coordinated to the quasi-2D HP surface improve the stability of the HP lattices, as it can act as a protection layer against environmental stressors (e.g., oxygen and moisture) .