applications, especially for fi eld-effect transistors (FETs) and sensors. [3][4][5][6] However, Klein tunneling in graphene and the related electron confi nement represent a real barrier to the development of graphene-based transistors, which results in a lack of band gap and the inability to confi ne electrons. [ 7 ] Therefore, although high mobility and high current are essential for high-frequency applications, this intrinsically high off-state current and low on/off ratio hinder the potential applications of graphene in FETs operated at room temperature.Numerous efforts have been devoted to inducing a band gap in graphene by chemical modifi cation, [8][9][10] the application of a perpendicular electric fi eld to bilayer graphene, [11][12][13] and other methods. [ 14 ] Nevertheless, these methods are uncontrollable and the as-constructed devices usually exhibit poor electronic performance. The fabrication of nanostructured graphene can be a quite effective way to introduce a bandgap. [ 15 ] Generally, nanostructured graphene refers to a graphene structure of intermediate size between microscopic and molecular, in which one dimension must be at the nanoscale, including graphene nanoribbons (GNRs), graphene nanomeshes, graphene nanodisks, graphene quantum dots, graphene nanoheterostructures, and so on. Among those graphene nanostructures, GNRs are the most popular and potentially useful ones for electronic applications; therefore, we will mainly concentrate on the progress made in GNRs. The narrowing of graphene fi lm into stripes with widths <10 nm was studied both theoretically and experimentally to create an energy band in the electronic structure of graphene due to quantum confi nement, which is the most effective way to open the band gap of graphene. In fact, the band gap is determined by the states of the edge and the width of the nanoribbon. [ 15 ] Tight binding (TB) calculations predict that GNRs terminated with 'armchair' edges can be either metallic or semi-conducting depending on their widths. Nanoribbons terminated with 'zigzag' edges are always metallic regardless of their widths. In order for the GNRs to open band gaps of a similar order as commonly used semiconducting materials (e.g. Si (1.14 eV), GaAs (1.43 eV)) widths of less than 2 nm are likely to be necessary. [ 16 ] Therefore, as the fi rst step to implement the electronic applications, nanostructured graphene must be directly synthesized Due to graphene's exceptional electronic properties, strong efforts are being made to push forward its nanoelectronic applications. However, the gapless band structure of truly 2D graphene makes it unsuitable for direct use in graphene-based fi eld-effect transistors (FETs), which is one of the most widely discussed graphene applications in electronics. Therefore, in order to accomplish graphene's applications in semiconducting nanoelectronics, it is necessary to produce nanostructured graphene with suffi ciently narrow characteristic width, thus introducing further confi nement and opening a reasonably la...