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Two-dimensional (2D) molybdenum disulfide (MoS 2 ) nanosheets were synthesized to anchor onto the surfaces of directly grown one-dimensional (1D) carbon nanotubes (CNTs) on fluorinated tin oxide (FTO) glass. This three-dimensional (3D) vertically aligned hybrid nanoarchitecture was used in Pt-free counter electrodes (CEs) for dye-sensitized solar cells (DSSCs). The prepared 2D MoS 2 nanosheets, with exposed layers, provided a great deal of edge-plane catalytically active sites for I 3 − reduction. The directly grown 1D CNTs provide an attractive template that offers a large surface area to promote the loading of 2D MoS 2 nanosheets for enhancing electrochemical activity. The CNTs directly grown on the FTO substrate provided a high-speed pathway that promoted charge transport and transfer, resulting in a lower electron lifetime that increased the exchange current density and reduced the charge-transfer resistance. The DSSCs assembled with the 3D vertically aligned MoS 2 /CNT hybrid nanoarchitecture CE achieved a power conversion efficiency of 7.83%, 9.5% higher than that of a cell prepared with a Pt film CE (7.15%). [ABSTRACT FROM AUTHOR]