Laser is used to produce graphene nanoribbons (GNRs) by unzipping carbon nanotubes (CNTs). It is found that laser can not only unzip CNTs, but also join GNRs through covalent reconnections. Because the CNTs are aligned in a freestanding CNT sheet, the laser irradiation process results in a freestanding GNR network. Experimental results show that the expected results can be achieved by controlling the delivery of laser beam energy to the sheet. Moreover, this process is a solid-state process and a scalable manufacturing process.