Abundant and renewable solar light is an ideal resource for the industrial application of TiO2 photocatalysis in environmental purification. Over the past decades, the pursuit for visible-light photocatalysts with low cost, simple process, and high efficiency remains a challenging task. Here, we report a novel organic-inorganic nanohybrid photocatalyst (conjugation-grafted-TiO2) by chemically grafting conjugated structures onto the surfaces of TiO2 nanoparticles through controlled thermal degradation of the coacervated polymer layer. The interfacial C-O-Ti bonds between TiO2 and conjugated structures can act as the pathway to quickly transfer the excited electrons from conjugated structures to TiO2, therefore contribute to high visible-light photocatalytic efficiency. Our findings provide an economic route to prepare the conjugation-grafted-TiO2 nanohybrid, and develop a routine to improve the photocatalytic efficiency of organic-inorganic hybrid materials through the interfacial interaction.