Atmospheric aerosols play a crucial role in Earth’s climate system, yet their spatio-temporal distribution, particularly in the free troposphere (FT) and upper troposphere–lower stratosphere (UTLS), remains poorly constrained, a major source of uncertainty in estimates of aerosol radiative forcing. To address this, we perform ECHAM/MESSy Atmospheric Chemistry (EMAC) model simulations with a newly developed setup, bridging the tropospheric and stratospheric regimes. Model output is evaluated against a comprehensive suite of observations of aerosol mass, number concentrations, and optical properties, showing good agreement across vertical layers and most geographical regions. The evaluated simulations provide a unified description of global distributions of key aerosol species, their composition, and number concentrations from the Earth's surface to the stratosphere. Simulated aerosol mass exhibits a global minimum between 400 and 200 hPa, marking the transition between FT and UTLS, with particle numbers peaking at similar altitudes or slightly higher in the tropics. Primary particles contribute less than 3.5 % to aerosol mass in the stratospheric overworld up to 10 hPa, substantially less than suggested by previous modelling studies and in closer agreement with recent observations. Stratospheric aerosol mass is dominated by sulfate, with a notable contribution (~15 %) from secondary organic aerosol throughout the global lower stratosphere. This work provides new constraints on aerosol distributions in the FT and UTLS, which remain underrepresented in global modelling studies, and enables future research on aerosol-climate interactions in this critical atmospheric regime.