Ultrathin nanostructures have attracted much attention in recent years due to their predictable novel properties and various potential applications. The improvement in synthetic skills has led to many successful syntheses of nanostructures including zerodimensional (0D) nanoclusters, one-dimensional (1D) nanowires, two-dimensional (2D) nanosheets and other higher-level complex nanostructures, where cluster-assembly of primary nanocrystals is a common process. In this review, progress in ultrathin nanocrystals in the last decade and several important factors in the growth mechanisms are covered. By giving examples of cluster assembly from 1D to 3D nanostructures, the utility of cluster assembly in the synthesis of new materials has been demonstrated. The improvement in synthetic skills has led to many successful syntheses of nanostructures including zerodimensional (0D) nanoclusters, one-dimensional (1D) nanowires, two- dimensional (2D) nanosheets and other higher-level complex nanostructures, where cluster-assembly of primary nanocrystals is a common process. In this review, progress in ultrathin nanocrystals in the last decade and several important factors in the growth mechanisms are covered. By giving examples of cluster assembly from 1D to 3D nanostructures, the utility of cluster assembly in the synthesis of new materials has been demonstrated.