The surface of a TiO2 photoelectrode was modified through a dip-coating process using an aqueous potassium nitrate (KNO3) solution to increase the power-conversion efficiency of dye-sensitized solar cells (DSSCs). The KNO3-modified TiO2 electrode was applied to the photoanode of the DSSCs. The DSSC with the KNO3-modified TiO2 electrode exhibited a short-circuit current (J(sc)) of 15.26 mA/cm2 and an open-circuit voltage (V(oc)) of 671 mV, compared with a J(sc) of 13.74 mA/cm2 and V(oc) of 654 mV for a reference device with a pristine TiO2 electrode. The results in combination with relevant data from electrochemical impedance spectroscopy, open-circuit voltage decay, and dark current measurements revealed that the modification of the TiO2 surface using the surface modifier (KNO3) led to a longer electron lifetime by the suppression of the charge recombination between injected electrons and I3- ions, resulting in an increase in both J(sc) and V(oc), compared with those of the reference device without surface modification.