Optically interfaced molecular spins are a promising platform for quantum sensing and imaging. Key for such applications is optically detecting coherent spin manipulation at room temperature. Here, using the photoexcited triplet state of organic chromophores (pentacene doped in p-terphenyl), we optically detect coherent spin manipulation with photoluminescence contrasts exceeding 15% at room temperature, both in a molecular crystal and thin film. We further demonstrate how multifrequency spin control could enhance such systems. These results open opportunities for room-temperature quantum sensors that capitalize on the versatility of synthetic chemistry.