We present a versatile method, based on the electrostatic self-assembly of oppositely charged species onto sacrificial templates, for the preparation of nanotubes. Polymer and polymer composite nanotubes were prepared by the layer-by-layer (LbL) deposition of polyelectrolytes and/or a charged inorganic molecular precursor onto nickel nanorods, followed by removal of the core by dissolution. Surface charge reversal of the nanotubes was observed at the end of each deposition step, which facilitated the multilayer buildup. The precursor core−shell nanorods prepared and the resulting nanotubes obtained upon dissolution of the core were characterized using transmission electron microscopy. The LbL approach is facile, adaptable, and able to be performed from aqueous-based solutions, thereby opening new avenues for the preparation of a broad range of nanotubes with tailored composition and wall thickness.