In this work, wood apple leaves dye has been extracted, characterized, and examined as a potential photosensitizer for dye-sensitized solar cells (DSSCs). The dye was extracted in an ethanolic medium from the fresh wood apple leaves and characterized using thin-layer chromatography (TLC), ultraviolet-visible (UV-Vis), and Fourier transform infrared (FTIR) spectroscopy. The current density-voltage (J–V) characteristics measurements were performed on the two assembled DSSCs for 1–22 days using fresh and seven days old extracted dye. The characterization results revealed that the extracted dye mainly contains the compound of carotenoids (neoxanthin), chlorophyll a, chlorophyll b, and their derivative (pheophytin) with various functional groups. The J–V characteristics of DSSCs indicate that an open-circuit voltage and short circuit current density radically decrease with increasing time, thus degrading the efficiency of cells. A degraded DSSCs suffered from high defect recombination may be induced by Mg ions migrating from chlorophyll dye into DSSC. Therefore, the extracted dye may be used for energy harvesting from the wood apple leaves.