The membrane-templating method was successfully combined with electrodeposition and layer-by-layer assembly to create various multisegmented nanostructures composed of metal, polymers, synthetic and biological polyelectrolytes, and colloids. The electrochemical approach offers the control over the architectural parameters of the resulting structures (in particular the segment length and morphology), whereas the LbL adsorption technique permits to integrate nonconducting materials, including biomacromolecules, within the nanostructures. A supplementary degree of complexity can be reached by capping or loading the LbL nanotubes with colloidal particles. The ability to easily generate such hybrid anisotropic nanoparticles with spatially resolved chemical, physical, and biochemical functionalities is a boon for the synthesis of nanostructures, which is of tremendous importance for electronic, sensing, drug delivery, and modern biomedical and biotechnological applications.