A high-performance quantum dot-sensitized solar cell (QDSSC) is reported, which consists of a TiO2/CuInS2-QDs/CdS/ZnS photoanode, a polysulfide electrolyte, and a CuS counter electrode. The sensitization process involves attaching presynthesized CuInS2 QDs (3.5 nm) to a TiO2 substrate with a bifunctional linker, followed by coating CdS with successive ionic layer adsorption and reaction (SILAR) and ZnS as the last SILAR layer for passivation. This process constructs a sensitizing layer that comprises CdS nanocrystals, closely packed around the earlier-linked CuInS2 QDs, which serve as the pillars of the layer. The CuS counter electrode, prepared via successive ionic solution coating and reaction, has a small charge transfer resistance in the polysulfide electrolyte. The QDSSC exhibits a short-circuit photocurrent (Jsc) of 16.9 mA cm−2, an open-circuit photovoltage (Voc) of 0.56 V, a fill factor of 0.45, and a conversion efficiency of 4.2% under one-sun illumination. The heterojunction between the CuInS2 QDs and CdS extends both the optical absorption and incident photon conversion efficiency (IPCE) spectra of the cell to a longer wavelength of approximately 800 nm, and provides an IPCE of nearly 80% at 510 nm. The high TiO2 surface coverage of the sensitizers suppresses recombination of the photogenerated electrons. This results in a longer lifetime for the electrons, and therefore, the high Voc value. The notably high Jsc and Voc values demonstrate that this sensitization strategy, which exploits the quantum confinement reduction and other synergistic effects of the CuInS2-QDs/CdS/ZnS heterostructure, can potentially outperform those of other QDSSCs.