Modulating the structure of a photocatalyst at the molecular level can improve the photocatalytic efficiency and provides a guide for the synthesis of highly qualified photocatalysts. In this study, TiO 2 was modified by various organic compounds to form different TiO 2 -based hybrid photocatalysts. 1,10-Phenanthroline (Phen) is an organic material with delocalized π-conjugated systems. It was used to modify TiO 2 to form the hybrid photocatalyst Phen/TiO 2 . Furthermore, 1,10-phenanthrolin-5-amine (Phen-NH 2 ) and 1,10-phenanthroline-5-nitro (Phen-NO 2 ) were also used to modify TiO 2 to form NH 2 -Phen/TiO 2 and NO 2 -Phen/TiO 2 , respectively. The samples of TiO 2 , Phen/TiO 2 , NO 2 -Phen/TiO 2 , and NH 2 -Phen/TiO 2 were carefully characterized, and their photocatalytic performance was compared. The results indicated that the photocatalytic efficiency followed the order of NH 2 -Phen/TiO 2 > NO 2 -Phen/TiO 2 > Phen/TiO 2 > TiO 2 . It could be found that modifying TiO 2 with different organic compounds containing delocalized π-conjugated systems could enhance the photocatalytic ability; furthermore, the level of this enhancement could be modulated by different delocalized π-conjugated systems.