© 2019 The Chemical Society of Japan A novel bisurea compound showed columnar liquid crystal phases possessing a new functionality, polarity-adjustability. Its molecular packing structures were analyzed by X-ray diffraction (XRD), and its polarity switching behavior and magnitude of the polarity were examined by electro-optic and second harmonic generation (SHG) experiments, respectively. As a result, it was revealed that the macroscopic polarity gradually increased with every ON/OFF cycle in SHG experiment applying an electric field. This strongly suggests that the anti-parallel hydrogen bonding network in each of the columns is reconstructed to syn-parallel by applying the electric field intermittently. Furthermore, it was confirmed that the reconstructed network mostly remained even once the temperature was raised to its isotropic state.