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Environmentally friendly natural dye-sensitized solar cells based on TiO2 nanorod arrays are sensitized using extracts of Radix Ophiopogonis fruits and Chinese purple yams as natural sensitizers. Compared with conventional natural dye-sensitized solar cells based on nanoporous TiO2 anodes, improved short-circuit photocurrent densities are recorded (from 3.5 mA/cm 2 to 5 mA/cm 2 and from 2.7 mA/cm 2 to 5.2 mA/cm 2 respectively) for solar cells using the TiO2 nanorod arrays. The best power conversion efficiencies obtained are 1.2% and 1.15% for solar cells sensitized by extracts of Radix Ophiopogonis fruits and Chinese purple yams, indicating increases of 155% and 91% compared with those based on nanoporous TiO2 films. These results indicate that the combination of TiO2 nanorod arrays and natural dyes may provide an efficient and stable structure for natural dye-sensitized solar cell applications.