A series of carbon nanohorns (CNHs) constituted by the aggregation of about 2000 individual conical graphene tubes (diameters from 2 nm to 5 nm and a length of 40–50 nm) that have been modified with dyes of two, three, or four terthienyl groups has been prepared by adsorbing the corresponding dye on the CNH. Persistent inks in o-dichlorobenzene (o-DCB) of these dye-CNH conjugates were obtained by laser irradiation of o-DCB suspensions of the dye-CNH solids. These inks were used in combination or not with N719 dye for the preparation of dye-sensitized solar cells (DSSC) of TiO2. It was measured that the terthienyl dye with the largest conjugation deposited on the CNH additively increased the performance of an analogous TiO2 cell from an efficiency of 4.07% to 6.24%. This result shows the potential of dye-modified CNHs as additives in the construction of more efficient DSSCs.