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With steadily rising CO2 concentrations in the ambient air and fast-changing concretecompositions with reduced clinker contents, the availability of reliable and accelerated concrete car-bonation tests is of crucial importance to design durable structures. This paper focuses on the effectsof moisture under accelerated conditions and the effects of different CO2 exposure conditions. Mor-tar prisms incorporating three different cement types were cured and stored at either 50% or 65%relative humidity (RH). Afterwards, the prisms were carbonated at different ambient humidities(50, 57 and 65%), different CO2 concentrations (0.04, 1 and 3 vol.%) and complemented by a seriesof tests at increased gas pressure (2 barg). High-resolution test methods were used to explain theunderlying carbonation mechanisms. The results show that pre-conditioning for two weeks—ascurrently suggested by the European Standard—seems to be too short because the initial inner mois-ture content severely affects the carbonation rate. Relative humidity during carbonation of 57% ledto higher carbonation rates compared to 50% and 65%. In addition, climate data needs to be period-ically (preferably permanently) recorded in research experiments and in laboratory testing to ensurefair interpretation of experimental results.