The formation of vertically aligned single-crystalline silicon nanostructures via "self-organized" maskless etching in Ar+H(2) plasmas is studied. The shape and aspect ratio can be effectively controlled by the reactive plasma composition. In the optimum parameter space, single-crystalline pyramid-like nanostructures are produced; otherwise, nanocones and nanodots are formed. This generic nanostructure formation approach does not involve any external material deposition. It is based on a concurrent sputtering, etching, hydrogen termination, and atom/radical redeposition and can be applied to other nanomaterials. (C) 2009 American Institute of Physics. [doi:10.1063/1.3232210]