Deterministic organization of nanostructures into microscale geometries is essential for the development of materials with novel mechanical, optical, and surface properties. We demonstrate scalable fabrication of 3D corrugated carbon nanotube ((NT) microstructures, via an iterative sequence of vertically aligned (NT growth and capillary self-assembly. Vertical microbellows and tilted microcantilevers are created over large areas, and these structures can have thin walls with aspect ratios exceeding 100:1. We show these structures can be used as out-of-plane microsprings with compliance determined by the wall thickness and number of folds.