Quasi-solid state dye-sensitized solar cells (DSSC) having bilayer structure were made by using nanocrystalline anatase-rutile TiO2 to enhance the photovoltaic performance. The bilayer structures were coated to FTO glass using doctor blade technique with total active area of 0.4 cm2. Cyanidin dye extracted from mangosteen pericarp was used as photosensitizer. Bilayer anataseanatase was formed with surface area of 99.9 m2/g and pore volume of 0.23 cc/g while anataserutile structure has surface area of 103.5 m2/g and pore volume of 0.21 cc/g. Overall energy conversion efficiencies under illumination of 10 mW/cm2 of 0.461% and 0.1365% were achieved for DSSC employing anatase-anatase and anatase-rutile TiO2 structure, respectively. Both efficiencies were higher than that of monolayer anatase and rutile TiO2 structure whose efficiencies in the range of 0.02% to 0.037%. The photocurrent action spectra of bilayer structures performed high efficiency spectrum in the wavelength range of 420 - 480 nm owing to cyanidin effect of dye.