The paper demonstrates room-temperature optically detected coherent control of molecular spins, specifically in pentacene doped with para-terphenyl. The authors achieve high photoluminescence contrasts (exceeding 10%) and microsecond coherence times at room temperature. They show that coherent control of multiple triplet sublevels can significantly enhance optical spin contrast and extend this functionality to a thermally evaporated thin film, maintaining high photoluminescence contrast and coherence times. These results open up opportunities for room-temperature quantum technologies, particularly in sensing and imaging applications, where the chemical tunability and versatile deposition techniques of organic chromophores are advantageous. The study highlights the potential for chemically tailored molecular platforms to achieve advanced detection capabilities, such as magnetic and electric field sensing, temperature measurement, and structural analysis of biomolecules.The paper demonstrates room-temperature optically detected coherent control of molecular spins, specifically in pentacene doped with para-terphenyl. The authors achieve high photoluminescence contrasts (exceeding 10%) and microsecond coherence times at room temperature. They show that coherent control of multiple triplet sublevels can significantly enhance optical spin contrast and extend this functionality to a thermally evaporated thin film, maintaining high photoluminescence contrast and coherence times. These results open up opportunities for room-temperature quantum technologies, particularly in sensing and imaging applications, where the chemical tunability and versatile deposition techniques of organic chromophores are advantageous. The study highlights the potential for chemically tailored molecular platforms to achieve advanced detection capabilities, such as magnetic and electric field sensing, temperature measurement, and structural analysis of biomolecules.