Achieving high surface coverage of the colloidal quantum dots (QDs) on TiO2 films has been challenging for quantum dot-sensitized solar cells (QDSCs). Herein, a general surface engineering approach was proposed to increase the loading of these QDs. It was found that S2− treatment/QD re-uptake process can significantly improve the attachment of the QDs on TiO2 films. Surface concentration of the QDs was improved by ∼60%, which in turn greatly enhances light absorption and decreases carrier recombination in QDSCs. Ensuing QDSCs with optimized QD loading exhibit a power conversion efficiency of 3.66%, 83% higher than those fabricated with standard procedures.