The design of highly efficient sensitizers is one of the most significant areas in dye-sensitized solar cell (DSSC) research. We have studied a series of benzothiadiazole-based D-π-π-A organic dyes, putting emphasis on the influence of the donor moiety on the DSSC’s efficiency. Using linear response time-dependent density functional theory (TDDFT) with the CAM-B3LYP functional different donor groups were characterized in terms of electronic absorption spectra and key photovoltaic parameters. As a reference a dye has been considered which has a benzothiadiazole fragment linked via thiophene rings to a diphenylamine donor and a cyanoacrylic acid acceptor. The different systems are first studied in terms of individual performance parameters, which are eventually aggregated into the power conversion efficiency. Here only the amino-substituted species shows a modest increase, whereas the dimethylamino case even shows a decrease.