With the rising food demands from the future world population, more intense agricultural activities are expected to cause substantial perturbations to the global nitrogen cycle, aggravating surface air pollution and imposing stress on terrestrial ecosystems. Much less studied, however, is how the terrestrial ecosystem changes induced by agricultural nitrogen deposition may modify biosphere–atmosphere exchange and further exert secondary feedback effects on global air quality. Here we examined the responses of surface ozone air quality to terrestrial ecosystem changes caused by year 2000 to year 2050 changes in agricultural ammonia emissions and the subsequent nitrogen deposition by asynchronously coupling between the land and atmosphere components within the Community Earth System Model framework. We found that global gross primary production is enhanced by 2.1 Pg C yr−1, following a 20 % (20 Tg N yr−1) increase in global nitrogen deposition by the end of the year 2050 in response to rising agricultural ammonia emissions. Leaf area index was simulated to be higher by up to 0.3–0.4 m2 m−2 over most tropical grasslands and croplands and 0.1–0.2 m2 m−2 across boreal and temperate forests at midlatitudes. Around 0.1–0.4 m increases in canopy height were found in boreal and temperate forests, and there were ∼0.1 m increases in tropical grasslands and croplands. We found that these vegetation changes could lead to surface ozone changes by ∼0.5 ppbv (part per billion by volume) when prescribed meteorology was used (i.e., large-scale meteorological responses to terrestrial changes were not allowed), while surface ozone could typically be modified by 2–3 ppbv when meteorology was dynamically simulated in response to vegetation changes. Rising soil NOx emissions, from 7.9 to 8.7 Tg N yr−1, could enhance surface ozone by 2–3 ppbv with both prescribed and dynamic meteorology. We, thus, conclude that, following enhanced nitrogen deposition, the modification of the meteorological environment induced by vegetation changes and soil biogeochemical changes are the more important pathways that can modulate future ozone pollution, representing a novel linkage between agricultural activities and ozone air quality.