Giant birefringence optical crystals play a pivotal role in the realm of advanced polarization optical devices. Large π-conjugated organic molecular crystals, renowned for their high polarizability, have emerged as an exemplary option for crafting optically anisotropic materials. In a bid to meticulously regulate the spatial configuration of these molecules, scientists have incorporated metal nodes to construct metal-organic frameworks that inherently possess conductivity. Although these frameworks harbor the material attributes with the potential to trigger immense optical anisotropy responses, conductive metal-organic frameworks frequently exhibit a tendency to tightly stack π ligands in an effort to optimize charge transport. This stacking behavior subsequently leads to robust interlayer coupling, which, in turn, substantially diminishes the observable optical anisotropy of the π ligands in macroscopic crystals.