Recent advances in modification engineering of graphene nanoribbons prepared via on‐surface synthesis are comprehensively reviewed. The varieties of graphene nanoribbons (GNRs) with narrow widths and specific edge/backbone structures and the electrical applications are presented. The GNR preparation strategy holds a bright future in both tailoring their bandgaps and the ultimate applications. Abstract 1D graphene nanoribbons (GNRs) have a bright future in the fabrication of next‐generation nanodevices because of their nontrivial electronic properties and tunable bandgaps. To promote the application of GNRs, preparation strategies of miscellaneous GNRs have to be developed. The GNRs prepared by top‐down approaches are accompanied by uncontrolled edges and structures. In order to overcome the difficulties, bottom‐up methods are widely used in the growth of various GNRs due to controllability of GNRs’ features. Among those bottom‐up methods, the on‐surface synthesis is a promising approach to prepare GNRs with distinct widths, edge/backbone structures, and so forth. Therefore, modified engineering of the GNRs prepared via on‐surface synthesis is of great significance in controllable preparation of GNRs and their potential applications. In the past decade, there have been a lot of reports on controllable preparation of GNRs using on‐surface synthesis approach. Herein, the advances of GNRs grown via on‐surface growth strategy are described. Several growth parameters, the latest advances in the modification of the GNR structure and width, the GNR doping/co‐doping with heteroatoms, a variety of GNR heterojunctions, and the device application of GNRs are reviewed. Finally, the opportunities and challenges are discussed.

Published in: "Advanced Materials".