Even though many organic dyes have been reported as photoinitiators/photosensitizers for free radical polymerization in the literature, the design and development of novel photoinitiating systems based on organic dyes adaptable for visible light irradiation, for example, 405 nm LED and sunlight still remains challenging. Recently, major achievements in the development of high‐performance photoinitiating systems based on organic dyes as light‐harvesting compounds and their uses as photoinitiators for photopolymerization under visible‐light irradiation have clearly emerged, giving rise to abundant literature. In this review, an overview of the recently synthesized chromophores belonging to various families of organic dyes and used as photoinitiators of polymerization during the 2018–2021 period are presented and classified. Recent works have resulted in the development of new chromophores exhibiting remarkable visible light absorption properties and excellent photoinitiation abilities upon irradiation with LEDs and/or sunlight in free radical photopolymerization processes. These developments notably indicate that sunlight has the advantages of being a cheap, unlimited, broad emission spectrum, and energy‐saving light source capable to be an efficient substitute to artificial light sources. The newly developed dye‐based photoinitiating systems designed to initiate visible‐light‐induced photopolymerization processes are likely to expand the scope of application of photopolymerization in modern sciences and technologies.