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1. Arthropod assemblages form a fundamental part of terrestrial ecosystems, underpinning ecosystem processes and services. Yet, little is known about how invertebrate communities, as a whole, respond to climatic and atmospheric changes, including predicted increases in carbon dioxide concentrations (CO2). 2. To date, woodland Free Air CO2 Enrichment (FACE) studies have focused entirely on northern hemisphere managed plantations. We manipulated atmospheric CO2 in a mature, native Eucalyptus woodland (0.15 ha, >32 000 m3) in Australia, using the Eucalyptus FACE (‘EucFACE’) facility. We used three complementary sampling methods (vacuum sampling, pitfall and sticky trapping) to record invertebrate abundances under ambient and elevated levels of CO2 (400 versus 550 ppm). 3. Based on the collection of over 83 000 invertebrates, we found significant declines in the overall abundance of ground-dwelling (14.7%) and aerial (12.9%) arthropods under elevated CO2, with significant decreases in herbivore, omnivore, scavenger and parasitoid functional groups. Even though several groups showed varying declines in abundance, elevated CO2 did not measurably affect community composition. 4. The results of the present study indicate that atmospheric CO2 levels predicted within the next 35 years may cause declines in arthropod abundances in Eucalyptus woodland. Declines found in several functional groups suggest that elevated atmospheric CO2 has the potential to affect ecosystem processes, possibly including nutrient cycling by herbivores and omnivores, as well as biocontrol by parasitoids.