order to explore the influence of diverse acceptors with varying amounts of electron withdrawing groups on the organic dye in dye-sensitized solar cell (DSCs), a series of JF419 organic analogues with several cyano groups (CN) on acceptor were engineered. By performing theoretical studies on these investigated dyes and the corresponding dye/(TiO2)(38) complexes, two benzoic acid units (benzothiadiazole benzoic acid and vinyl benzoic acid) with more -CNs were identified as alternative acceptors for DSCs. Particularly, S3 and S5 dyes exhibited impressive red-shift in spectra (ca. 77 nm for S3 and 48 nm for S5 compared with JF419), more accessible charge separation state and large driving force for dye regeneration (Delta G(reg) = 0.51 eV for S3 and Delta G(reg) = 0.61 eV for S5). According to quantifying the charge transfer (CT) on semiconductor surface, it found that the growing electron withdrawing groups on acceptor can strengthen the interaction between dyes and TiO2 and provide favorable conditions for electron injection. A brilliant balance between the electron injection time (tau = 6.8 fs for S3 and tau = 7.3 fs for S5) and the electron-hole recombination distance (r = 20.5 angstrom for S3 and r = 19.2 angstrom for S5) could be acquired for S3 and S5 dyes. Synthetically, introducing electron withdrawing groups on acceptor for organic dyes is a valid approach for gaining great performance of DSCs.