One dimensional (1D) nanomaterials have attracted a lot of attention owing to its intriguing performance. However, cost-efficient macroscopic assembly of 1D nanomaterials into free-standing and well-aligned macroscopic structures that are anisotropic and highly ordered in microscopic appearance is still a challenge. Here, we report a general and versatile technology to directly assemble MoO3 nanobelts into macroscopic structures, including film and yarn, without using any extra functionalization agent or cross-linking agent. MoO3 nanobelts are close-packed as parallel arrays with longitudinal axes aligned perpendicular to the capillary force. Carrier mobility of aligned film along nanobelt axis and perpendicular directions are about 400 and 30 cm2/(V·s), respectively. The promising carrier mobility raised from its high-order alignment indicates potential application in thin film transistors. High degree order of assembled MoO3 yarn also enables large tensile strength of up to 120 MPa, which is superior to...