Natural dye extract of the saffron petal, purified by solid-phase extraction (SPE) technique, has been studied as a novel sensitizing dye to fabricate TiO2 nanoparticles-based dye-sensitized solar cells (DSSC). The extract was characterized using ultraviolet–visible (UV–Vis) and Fourier transform infrared (FTIR) spectroscopies to confirm the presence of anthocyanins in saffron petals. The typical current–voltage and the incident photon to current efficiency (IPCE) curves were also provided for the fabricated cell. The saffron petal extract exhibited an open-circuit voltage (Voc) of 0.397 V, short circuit current density (Jsc) of 2.32 mA/cm2, fill factor (FF) of 0.71, and conversion efficiency of 0.66%, which are fairly good in comparison with the other similar natural dye-sensitized solar cells. These are mainly due to the improved charge transfer between the dye extract of saffron petal and the TiO2 anode surface. Considering these results, it can be concluded that the use of saffron petal dye as a sensitizer in DSSC is a promising method for providing clean energy from performance, environmental friendliness, and cost points of view.