In this investigation, the chemical and microstructural characteristics of nanostructured AlFe intermetallic produced by high-energy ball milling have been explored. High purity elemental powders were used as the starting material. The ball milling was carried out at room temperature using a SPEX-8000 mixer/mill. The structure, morphology and compositions of the powders were obtained using X-ray diffraction patterns (XRD), scanning and transmission electron microscopy (STEM). High resolution electron microscopy observations have been used in the nanostructured materials characterization. The structural configurations have been explored through comparisons between experimental HREM images and theoretically simulated images obtained with the multislice method of the dynamical theory of electron diffraction.