Colloidal anisotropic semiconductor nanocrystals manifest polarized luminescence, high gain coefficient and improved charge transport, and show many advantages over isotropic spherical quantum dots in a variety of applications such as lighting and displays, lasering and catalysis. However, it is challenging to accomplish the controlled syntheses of both heavy-metal-free semiconductor nanocrystals and metal halide perovskite nanocrystals due to the narrow growth window parameters and extremely fast growth rate originated from the highly ionic nature of the materials, respectively. In this talk, I will elaborate how the size, morphology, composition and surface of such nanocrystals can be controlled and be further self-assembled into hierarchical architectures via regulating a broad scope of factors ranging from surface energy, monomers, additives, binding ligands to temperature from a physical perspective. The optical, electronic, and catalytic properties of these intriguing materials have been interpreted based on the structure-property relationships and their super performance in optoelectronics, catalysis and latent fingermark detections have been demonstrated.