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Al-based glassy alloys (metallic glasses) have been of great scientific and technological interest as a high specific strength and high corrosion resistant materials. However, the low glass-forming ability (GFA) is still a choke point that greatly influences the applications. In order to further comprehend the glass formation mechanism and investigate the possibility of enhancing the GFA, it is important to obtain the definite information on the atomic scale glassy structures in correlation with properties and to study the composition dependence of crystallization and properties of Al-based metallic glasses. The purpose of this paper is to summarize the structure characteristics and crystallization behavior in conjunction with alloy component in Al-based metallic glasses and to investigate the possibility of synthesizing an Al-based bulk metallic glass with better engineering performances. This may assist to learn the structural features systematically and understand the development and current status for Al-based metallic glasses.