Nonlinear optical materials whose optical properties change in accordance with an incident light intensity have attracted much attention. In particular, liquid crystals (LCs) can reversibly control their molecular orientation based on nonlinear optical effects. The doping of oligothiophene dye into LCs increases the light sensitivity. Further enhancement of the light sensitivity is still desired for practical applications. In this study, we investigated the effect of the host LC structure such as fluorinated LCs on the nonlinear molecular reorientation behavior, aiming to increase the sensitivity of the photoinduced molecular reorientation.