Here,we demonstrate a bottom-up approach for the fabrication of well-defined dimensional-crossover nano-architectures with high tunability using metal ions and organic molecules as building blocks [1-11].We succeeded in rationally constructing an assembly of square prism-shaped metal-organic nanotubes with aside of 2 nm.A uniform 1D channel is fabricated inside the tube,and H2O and alcohol can be selectively adsorbed.Its optical gap is about 0.76 eV of semiconductive region,and X-ray and theoretical studies revealed its unique electronic structure of CDW quartets.In addition,its electronic states can be successively controlled by exchanges of structural components and guest molecules.The results presented here demonstrate a rational route to the creation of nanotubes with high tunabilities of structures and electronic states,and might also offer valuable insights into multifunctional nanomaterials.