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 synparallel 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.