This study demonstrates room-temperature optically detected coherent control of molecular spins using organic chromophores, specifically pentacene doped in a para-terphenyl host. The system enables high-contrast optical spin manipulation with microsecond coherence times and ambient operation. The research shows that coherent control of multiple triplet sublevels can significantly enhance optical spin contrast, and extends optically detected coherent control to a thermally evaporated thin film, maintaining high photoluminescence contrast and coherence times. These results open opportunities for room-temperature quantum technologies that can be systematically tailored through synthetic chemistry. The study highlights the potential of molecular spin systems for quantum technologies, offering advantages such as chemical versatility and the ability to interface with various targets. The research demonstrates the use of photoexcited triplet states of organic chromophores for room-temperature optically detected coherent control, with applications in quantum sensing and imaging. The system allows for high sensitivity optical detection, enabling structural analysis of individual biomolecules and ultrasensitive fluorescent assays. The study also shows that molecular spin systems can be used for spin-based quantum sensors, with the potential for high-density ensemble-based sensing. The research demonstrates the use of molecular spin systems for quantum metrology, with promising results in terms of sensitivity and coherence times. The study also highlights the potential for further optimization of these systems through synthetic chemistry and advanced control techniques. The results show that molecular spin systems can be used for quantum sensing with high sensitivity and coherence times, and that these systems can be tailored through synthetic chemistry. The study also highlights the potential for further optimization of these systems through synthetic chemistry and advanced control techniques. The research demonstrates the potential of molecular spin systems for quantum technologies, with applications in quantum sensing and imaging. The study also highlights the potential for further optimization of these systems through synthetic chemistry and advanced control techniques.This study demonstrates room-temperature optically detected coherent control of molecular spins using organic chromophores, specifically pentacene doped in a para-terphenyl host. The system enables high-contrast optical spin manipulation with microsecond coherence times and ambient operation. The research shows that coherent control of multiple triplet sublevels can significantly enhance optical spin contrast, and extends optically detected coherent control to a thermally evaporated thin film, maintaining high photoluminescence contrast and coherence times. These results open opportunities for room-temperature quantum technologies that can be systematically tailored through synthetic chemistry. The study highlights the potential of molecular spin systems for quantum technologies, offering advantages such as chemical versatility and the ability to interface with various targets. The research demonstrates the use of photoexcited triplet states of organic chromophores for room-temperature optically detected coherent control, with applications in quantum sensing and imaging. The system allows for high sensitivity optical detection, enabling structural analysis of individual biomolecules and ultrasensitive fluorescent assays. The study also shows that molecular spin systems can be used for spin-based quantum sensors, with the potential for high-density ensemble-based sensing. The research demonstrates the use of molecular spin systems for quantum metrology, with promising results in terms of sensitivity and coherence times. The study also highlights the potential for further optimization of these systems through synthetic chemistry and advanced control techniques. The results show that molecular spin systems can be used for quantum sensing with high sensitivity and coherence times, and that these systems can be tailored through synthetic chemistry. The study also highlights the potential for further optimization of these systems through synthetic chemistry and advanced control techniques. The research demonstrates the potential of molecular spin systems for quantum technologies, with applications in quantum sensing and imaging. The study also highlights the potential for further optimization of these systems through synthetic chemistry and advanced control techniques.