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Ammonium sulfate [(NH4)2SO4] deposition and elevated ozone (O3) concentrations may negatively affect plants and trophic interactions. This study aimed to evaluate for the first time the interactive effects of high (NH4)2SO4 load and elevated O3 levels on cauliflower (Brassica oleracea L.) under field conditions. Cauliflower seedlings were treated with 0 (AS0) or 50 (AS50) kg ha−1 (NH4)2SO4 and exposed to ambient (AOZ, ≈20 ppb) or elevated (EOZ, ≈55 ppb) O3 for about one month, in a Free Air O3 Concentration Enrichment (FACE) system. The oligophagous diamondback moth (Plutella xylostella Linnaeus, 1758) showed a clear preference towards the seedlings treated with AS50, which intensively grazed. Plant-herbivore interactions were driven by (NH4)2SO4 availability, rather than O3, via increased nitrogen content in the leaves. Further laboratory bioassays were followed to confirm the validity of these observations using polyphagous Eri silkmoth larvae (Samia ricini) as a biological model in a standardized experimental setup. Choice assays, where larvae could select leaves among leaf samples from the different experimental conditions, and no-choice assays, where larvae could graze leaves from just one experimental condition, were conducted. In the choice assay, the larvae preferred AS50-treated leaves, in agreement with the field observations with diamondback moth. In the no-choice assay, larval body mass growth was inhibited when fed with leaves treated with EOZ and/or AS50. Larvae fed with AS50-treated leaves displayed increased mortality. These observations coincide with higher NO3 and Zn content in AS50-treated leaves. This study shows that plant-herbivore interactions can be driven by (NH4)2SO4 availability, independently of O3, and suggests that high N deposition may have severe health implications in animals consuming such plant tissues. Key message: Plant-herbivore interactions are driven by high (NH4)2SO4 availability, independently of O3.