Bias-Free Water Splitting In article number 2204495, Xin Tong, Lianzhou Wang, Zhiming M. Wang, and co-workers develop a quantum dots (QDs)-based photoelectrochemical (PEC) device comprised of tandem Zn-doped CuInS2 QDs-decorated metal oxide electrodes (BiVO4 and Cu2O) for bias-free solar water splitting. Both the ligands capped on QDs and QDs-electrode heterojunctions are rationally engineered to promote the photo-induced charge transfer in the PEC system, delivering a solar-to-hydrogen efficiency of 0.65% with excellent stability.