Organic dyes that consist of a [2.2]paracyclophane moiety between a triphenylamine donor group and a cyanoacrylic acid acceptor group have exhibited considerably high values of open-circuit voltage (Voc) in the range of 0.69–0.74V. In an experiment that involved using an ion liquid electrolyte (E2 electrolyte), the values of Voc were increased to 0.03–0.04V because of a decrease in the concentration of LiI. A typical device demonstrated a maximal incident photon-to-current conversion efficiency (IPCE) of 60% in the region of 350–475nm, a short-circuit photo current density (Jsc) of 8.80mAcm−2, an open-circuit photovoltage (Voc) of 0.74V, and a fill factor (FF) of 0.65, corresponding to an overall conversion efficiency of 4.24% of CPG2b. The photophysical properties were analyzed using a time-dependent density functional theory (TDDFT) model with the M062X functional.