This work evaluates the suitability of the Al64Cu25Fe11 compound to enhance spectral solar absorption when replacing the mesoporous layer material of dye-sensitized solar cells. The compound is produced by high-energy ball milling, a mechanical alloying technique that ensures extensive inter-diffusion of the elemental components, while heat treatment that ensues promotes the appearance and growth of an icosahedral phase that possesses attractive microstructural and optical properties. These properties, along with electrical ones of Al-Cu-Fe compound, are compared with those of titania, a prominent mesoporous material in solar cell construction in an attempt to replace the scarce and expensive titania. A full array of microstructural, thermal, electrical, and optical analysis of the mechanically alloyed compound is presented to investigate and support this goal. Copyright (c) 2015 John Wiley & Sons, Ltd.