Efficient photogenerated charge separation is needed for potential solar energy conversion and storage. Herein, we present the preparation and characterization of an optically active anthracence-based molecule 4,4′-(anthracene-2,6-diylbis(azanediyl))bis(4-oxobutanoic acid) (ABDA), whose coupling with TiO2 has been proven useful in the pursuit of enhanced photoelectrochemical (PEC) performance. Ultraviolet-visible absorption spectroscopy and PEC measurements indicated that the ABDA/TiO2 composite has extended the light absorption of TiO2 to the visible region and efficiently increased the charge separation. The photocurrent of ABDA/TiO2 is 1.8 times higher than that of pristine TiO2. This study has provided a method for the development of functionalized TiO2 with enhanced PEC behaviour for energy conversion applications.