An electrostatic forces (EF)-controlled electric unzipping method was developed for producing graphene nanoribbon (GNR) from both single- (SWCNT) and multi-walled carbon nanotubes (MWCNT). Experimentally, an electrostatic generator was employed by taking its two electrodes with opposite charges to alternatively link to the metal vessel and the CNT/water solution to form two oppositely electric cycles corresponding to the EF in enhancement or reduction, respectively. Transmission electron microscopy images showed that this applied method can unzip both the SWCNT and MWCNT into relative GNRs. During the EF-controlled electric unzipping process, the concentration increases and EF-controlled in reduction model can produce GNRs with enhanced width and quality.