Fatty-imidazolinium electrolytes, waste graphite dispersed composite electrolytes like cocktails (1,3-methyl octyl-1,2,3benzotiazolium acetate-cis-oleyl-imidazolinium iodide), and graphite exfoliation using cis-oleyl-imidazolinium acetate have been studied to enhance the efficiency of a newly developing dye-sensitized solar cells (DSSCs). The DSSCs were fabricated in a sandwich structure and characterized using Solar Simulator. The graphite exfoliation was conducted by sonication and microwave energy, as well as the electrochemical method. Cis-oleyl-imidazolinium iodide efficiency (0.53%) was highest than stearyl-imidazolinium iodide and palmityl-imidazolinium iodide because cis-oleyl-imidazolinium iodide has a double bond and the longest alkyl chain which triggered a self-assembly structure formation and increased the rate of I -/I 3transport in cells. Then, the efficiency of DSSCs-based composite electrolytes was in the range of 0.020-0.203%. Dispersion of 0.05% of the graphite results in efficiency enhancement of about 100%, but the greater fraction (0.10%) of the graphite causes a poor performance (lower efficiency), possibly due to interference of the internal electron transportation routes in the DSSC by insoluble graphite. After exfoliation, the conductivity of synthetic graphite (11.58 x 10 -1 S/cm), new battery graphite (9.32 x 10 -1 S/cm), and battery waste graphite (7.96 x 10 -1 S/cm) were increased respectively 10 times, 2 times, and 4 times from the graphite before exfoliation due to changes in crystallinity, the distance between layers, crystal size, formation of multilayer graphene, and the occurrence of π to π* transition. This enhancement of solar conversion efficiency can give a new contribution to the development of DSSC.