Progressive restrictions on the use of toxic chromate-based corrosion inhibitors present serious technical challenges. The most critical of these is the lack of non-toxic ‘green’ alternatives that offer comparable performance, particularly on corrosion-prone aluminium alloys such as the 2000 and 7000 series. In this study we used computational modelling methods to investigate the properties of a range of small organic, potentially safer inhibitors and their interactions with technologically relevant alloy surfaces. We have generated robust and predictive computational models of corrosion inhibition for a structurally related data set of organic compounds from the literature. Our studies have correlated molecular features of the inhibitor molecules with inhibition and identified those features that have the greatest impact on experimentally determined corrosion inhibition. This information can be used to drive guided decision making for in silico or experimental screening of molecules for their corrosion inhibition efficiency, while considering more carefully their environmental consequences.