Natural pigment can act as an inexpensive and biologically-friendly dye, which is fabricated on a TiO2/FTO substrate. Natural pigments promote the efficiency of the photoelectric conversion in water-based DSSC with the aqueous electrolyte of the Ce+4/+3 system. The open-circuit voltage (Voc) of natural pigment in water-based DSSC is 0.640 V. The short-circuit current (Isc) of natural pigment in water-based DSSC is 0.658 mA/cm2. The efficiency of the photoelectric conversion in water-based DSSC of natural pigment is up to 0.131%. The natural pigments in DSSC are potentially applicable to turning solar energy into environmentally-friendly energy.