GNRs can be readily produced by unzipping the nanotubes because CNT structure can be analogically considered as graphene sheets rolled up. This is a special 2D graphitic structure performing the exceptional properties. Due to the unique structure and the outstanding properties, GNRs have been used in a vast range of applications, including transistors, optical and microwave communication devices, biosensors, chemical sensors, electronic memory and processing devices, nano electromechanical systems, and composites. The morphology of the fiilms was observed by scanning electron microscopy (SEM), and the properties of graphene were characterized by Raman spectroscopy. The conductivity of the fiilms was measured by a semiconductor parameter measurement system. Raman spectroscopy showed that the Raman characteristics of graphene characterized by optimized process were enhanced. Laser energy and irradiation time were two important parameters for the preparation of graphene from carbon nanotubes. In this study, to open carbon nanotubes by laser, graphene nanoribbons were produced by excimer laser irradiation of carbon nanotubes thin films. The experimental results show that, with the laser energy 150 mJ, the carbon nanotubes are not opened while the connection is observed. With the energy 450 mJ, the carbon nanotubes can be effectively destroyed, and graphene strips can be partially opened to form. At this time, the conductivity of the fiilm reaches the maximum value. Due to the thermal accumulation effect, a large number of porous structures appear on the wall of carbon nanotubes.