The scalable syntheses of functional, porous nanostructures with tunable three-dimensional morphologies is a significant challenge with potential applications in chemical, electrical, electrochemical, optical, photochemical, and biochemical devices. As a result, several bio-enabled and synthetic approaches are explored in this work (with an emphasis on peptide-enabled deposition) for the generation of aligned nanotubes of nanostructured titania for application as electrodes in dye-sensitized solar cells and biofuel cells. As part of this work, peptide-enabled deposition was used to deposit conformal titania coatings onto porous anodic alumina templates under ambient conditions and near-neutral pH to generate aligned, porous-wall titania nanotube arrays that can be integrated into dye-sensitized solar cells where the arrays displayed improved functional dye loading compared to sol-gel-derived nanotubes. A detailed comparison between synthetic and bioorganic polyamines with respect to titania film properties deposition rate provided valuable information for future titania coating experimental design given specific applications. The development of template-based approaches to single-wall titania nanotube arrays led to the development of a new synthetic method to create aligned, multi-walled titania nanotube arrays. Lastly, peptide-enabled deposition methods were extended beyond inorganic mineral and used for enzyme immobilization by cross-linking the peptide with the multicopper oxidase laccase. Peptide-laccase hybrid enzyme coatings improved both the amount of enzyme adsorbed onto carbon nanotube “buckypaper” and allowed the enzyme to retain more activity upon immobilization onto the surface.