Molecular and supramolecular chirality have always played an important role in chemistry as life has developed around building blocks of specific handedness (L-amino acids and Dsugars), a phenomenon known as homochirality. This has enormous implications, for instance, in drug design as only one enantiomer of a particular compound will have the desired pharmacological effect. However, in recent years supramolecular chirality has shown tremendous potential for other technological applications, like optoelectronics, sensing, magnetism, information technology, and imaging. These applications typically require chromophoric groups that can easily absorb and emit light, and move energy or charge efficiently. The chirality in the material may be an intrinsic property of the chromophore, like in helicenes, or be imprinted by attaching a chiral substituent on an achiral chromophore. This molecular-scale chirality then influences the aggregation of the constituent units, leading to a chiral supramolecular assembly. However, the supramolecular structure is also influenced by the preparation method, which often leads to polymorphism within the same sample. Because of the nature of the technological applications of these materials, their characterization often relies on spectroscopic techniques based on the interaction with chiral light, i.e., circularly polarized light. The dominant techniques are electronic circular dichroism (ECD), which measures the difference in absorption between left and right circularly polarized light, and its emission analogue, circularly polarized luminescence (CPL). ECD is sensitive to both the intrinsic chiral nature of the chromophoric units as well as the supramolecular chirality of the assembly. CPL can provide important information about the structural reorganization of the material after absorption and charge transport dynamics. Furthermore, the intrinsic luminescence of the material may be a target property in and on itself, for instance, for the fabrication of circularly polarized-organic light emitting diodes (CP-OLEDs). 17, The application of these techniques relies on complementary theoretical simulations, which can help elucidate structure-property relations. However, while simulation of ECD and even CPL spectra are now routine for molecules thanks to robust and easy-to-use implementations of time-dependent density functional theory (TDDFT) and excited state energy gradients (which allow relatively reliable geometry optimizations of the first excited state), this is not the case for extended materials. In fact, most simulations for these materials are based on molecular clusters and excitonic models for the interaction between spatially separated chromophores. However, these approaches rely on significant assumptions, e.g. localized excitations and structural rigidity, that may not always be valid. Therefore, robust methods that are agnostic about the electronic response are desirable, for instance based on TDDFT with periodic boundary conditions (PBCs), but so far they are not commonly available. In this perspective, we discuss the theoretical quantities that need to be evaluated to simulate ECD and CPL spectra of oriented solid materials and the current state of the quantum mechanical methods to calculate these quantities. This work does not aim to provide a comprehensive review of the literature, but rather to discuss the challenges and the opportunities to develop computational tools for the simulation of ECD and CPL spectra for materials that are as reliable and accessible as for molecules. Such methods would provide invaluable guidance for the interpretation of experimental spectra and may help in the definition of rational design principles for the development of new materials with target chiroptical properties.