BackgroundThe cotton aphid, Aphis gossypii Glover (Hemiptera: Aphididae) is an important pest of cotton and horticultural crops globally. In China, smallholder farmers regularly intercrop cotton with garlic or onion. Aside from higher farm‐level revenue, cotton intercrops are typified by lower Aphis gossypii abundance than monocrops. So far, the mechanistic basis of this lowered pest pressure has not been empirically assessed.ResultsField trials showed that Aphis gossypii abundance is lower and (relative) abundance of aphid predators higher in early‐season cotton intercrops than in monocrops. Cage trials and Y‐tube olfactometer tests further indicated that garlic and onion volatiles repel Aphis gossypii alates. Electrophysiological bioassays and gas chromatography–mass spectrometry (GC–MS) identified two physiologically active volatiles, that is, diallyl disulfide and propyl disulfide from garlic and onion respectively. Next, behavioral tests confirmed that both sulfur compounds exert a repellent effect on alate Aphis gossypii.ConclusionGarlic and onion volatiles interfere with Aphis gossypii settling, but do not affect its main (ladybird) predators. Meanwhile, early‐season cotton/onion intercrops bear higher numbers of Aphis gossypii predators and fewer aphids. By thus unveiling the ecological underpinnings of aphid biological control in diversified cropping systems, our work advances non‐chemical management of a globally‐important crop pest. © 2023 Society of Chemical Industry.