<p>Circularly polarized luminescence (CPL) is a phenomenon where chiral molecules emit light with distinct left or right circular polarizations upon excitation. Unlike conventional luminescent materials, chiral materials produce light with inherent helicity, leading to unique applications in chiral opto-electronics, quantum technologies, and biophotonics. This review systematically explores the theoretical and computational foundations of CPL, focusing on the interplay between molecular chirality, transition dipole moments, and photoluminescence quantum yield. A major challenge in designing efficient CPL-active materials is optimizing the luminescence dissymmetry factor (<i>g</i>_lum) while maintaining high photoluminescence efficiency. This review comprehensively summarizes how first-principles computational methods, by establishing robust predictive frameworks, have significantly advanced the design of CPL molecules. Even though significant progress has been made in modeling the monomeric systems, the effective integration of first-principles calculations to describe the CPL in aggregated states remains an ongoing challenge. The review also highlights the promising synergy between computational models, experimental validation, and emerging data-driven techniques such as machine learning (ML) for guiding the design of novel high-performance CPL materials. In conclusion, further research is needed to overcome current computational limitations and develop more effective strategies for CPL material design.</p>