Al-Y-Fe amorphous and nanocrystalline alloys are characterized by a unique collection of diverse properties that are influenced by various factors, including heat treatment. In this paper, the effect of heat treatment on the structural changes and selected properties of Al-Y-Fe metallic glasses in the as-spun state is investigated. The structure of the Al88Y7Fe5 and Al88Y6Fe6 alloys was examined by X-ray diffraction (XRD) and Mössbauer spectroscopy (MS). The corrosion resistance of the samples was characterized using polarization tests in a 3.5% NaCl solution at 25 °C. The effect of sodium chloride on the surface was studied with scanning electron microscopy (SEM) and energy-dispersive spectroscopy (EDS). The magnetic properties of Al-based alloys were explored using a vibrating sample magnetometer (VSM). It was revealed that the tested alloys show better properties after annealing than in the as-spun state. The annealing of the Al88Y7Fe5 and Al88Y6Fe6 alloys in the temperature range of 200 to 300 °C improved the magnetic properties and corrosion resistance of these materials. After 3,600 s, the better EOCP values were recorded for the Al88Y6Fe6 and Al88Y7Fe5 alloys after annealing at 300 °C and 200 °C, adequately. On the basis of the polarization tests, it was concluded that the electrochemical properties are better for Al88Y6Fe6 alloys after annealing at 300 °C.