Aluminum, despite its abundance and low cost, is usually avoided for plasmonic applications due to losses in visible/infrared regimes and its interband absorption at 800 nm. Yet, it is compatible with silicon CMOS processes, making it a promising alternative for integrated plasmonic applications. It is also well known that a thin layer of native Al2O3 is formed on aluminum when exposed to air, which must be taken into account properly while designing plasmonic structures. Here, for the first time we report exploitation of the native Al2O3 layer for fabrication of periodic metal-insulator-metal (MIM) plasmonic structures that exhibit resonances spanning a wide spectral range, from the near-ultraviolet to mid-infrared region of the spectrum. Through fabrication of silver nanoislands on aluminum surfaces and MIM plasmonic surfaces with a thin native Al2O3 layer, hierarchical plasmonic structures are formed and used in surface-enhanced infrared spectroscopy (SEIRA) and surface-enhanced Raman spectrocopy (SERS) for detection of self-assembled monolayers of dodecanethiol. (Chemical Equation Presented). © 2014 American Chemical Society.