A possible way to valorize citrus peels and seeds, which are byproducts of the juice extraction industry, is to use them as natural antioxidants. The antioxidant activity of several citrus peel and seed extracts obtained either by methanol extraction (free phenolic compounds) or by alkaline hydrolysis (bound phenolic compounds) was tested in a model system based on accelerated citronellal oxidation. Generally, seeds possessed greater antioxidant activity than peels. The composition of all tested samples was studied by HPLC: methanol extracts are rich in flavones and glycosylated flavanones, whereas hydrolyzed extracts contain mainly phenolic acids and flavonols. The phenolic composition of some citrus peels and seeds was described for the first time. No clear relationship could be shown between the antioxidant activity and the phenolic composition of the extracts.