The anodization of metals through porous anodic alumina (PAA) matrix (PAA-assisted anodization) is used alternatively to nanoporous anodization or conventional nanofabrication methods for producing novel nanostructured metal oxides with improved characteristics. Enhancing properties of ZrO2 and HfO2 by nanostructuring possesses significant interest due to the active commercialization of these metal oxides. Nanostructuring ZrO2 and HfO2 by anodization is challenging because of early anodic-oxide crystallization and nearly zero cation transport number. These issues are addressed by a systematical investigation of anodizing behavior of Al superimposed on Zr or Hf layers. Reproducible PAA-assisted growth of ZrO2 nanostructures partially filling the pores of the PAA matrix is achieved for the first time. The PAA-embedded ZrO2 nanostructures demonstrate enhanced dielectric performance in a wide frequency range with low leakage current and high breakdown voltage, making them attractive for application in wet and hybrid electrolytic capacitors. The planarized films compatible with standard nanofabrication methods and comprising ZrO2 nanostructures fully filling the pores in the PAA matrix are synthesized by combining the PAA-assisted anodization of Zr with partial PAA dissolution. Such films are utilized in experimental MIM microcapacitors exhibiting low leakage current, high breakdown voltage, high energy density, low temperature coefficient of capacitance, and excellent capacitance-voltage linearity, which makes them perfect candidates for on-chip passive device integration. The PAA-assisted ZrO2 nanofilms are approbated for the first time to produce osteogenic bioceramic coatings. Such nanostructured ZrO2 bioceramic coatings can module cell-surface interactions and increase osteoblast mineralization 5-fold compared to flat ZrO2 anodic coating. The PAA-assisted nanostructured HfO2 films exhibit repeatable low-power eigh-wise bipolar resistive-switching properties, making them highly prominent as solid electrolytes in memristor applications. The PAA-assisted anodization of Hf combined with appropriate surface chemical modification is utilized for the first time for creating self-organized superhydrophobic, oil-repelling, visible light transparent, and antireflective nanostructured HfO2 coatings highly suitable for passivation of photovoltaic devices.