This review summarises the research work published in the last two decades on the use of natural compounds as corrosion inhibitors for aluminium and aluminium alloys in different solutions. Herein, plant extracts, gums, drugs, and oils have been considered as green corrosion inhibitors. The advantages and disadvantages of the methods used to obtain green corrosion inhibitors are presented. Additionally, the inhibition effectiveness of these corrosion inhibitors, including the techniques used to evaluate them and the respective inhibition mechanisms, are discussed. Finally, a critical evaluation is presented together with the outlook as regards possible future improvements.