Based on theoretical calculations, we studied four triphenylamine (TPA)-based dyes (namely D1-D4) incorporating electron-deficient thiadiazole derivatives as the π-spacer for the applications in dye-sensitized solar cells (DSSCs).The effects of the electron-deficient units on the spectra and electrochemical properties have been investigated by the combination of density functional tight-binding (DFTB), density functional theory (DFT), and time-dependent DFT (TDDFT) approaches.Compared with the model compound D0, which adopts a phenylene unit as the π-spacer, D1-D4 dyes display remarkably enhanced spectral responses in the red portion of the solar spectrum and possess desirable energetic properties once anchored on TiO2 surface. The newly constructed dyes D2, D3, and D4 demonstrate desirable energetic and spectroscopic parameters, and may lead to efficient metal-free organic dye sensitizers for DSSCs.