Simultaneous measurements of O 3 , CO, and ultrafine aerosol particles (UFP), conducted on board of a Boeing 767‐ER passenger aircraft flying from Sri Lanka to Germany (project CARIBIC), are used to study two‐way cross‐tropopause mixing near a subtropical tropopause fold. On the equatorward side of the fold, downward mixing of stratospheric air into the upper troposphere is identified by enhanced concentrations of O 3 and 14 CO. Very high UFP number concentrations of up to 1.5×10 4 cm −3 (STP) were encountered inside the poleward half of the fold. This accumulation of small particles is explained by recent extensive aerosol nucleation, most likely triggered by the mixing of stratospheric air with tropospheric air injected into the fold. Further, nine particle formation events were observed outside the fold which are attributed to isolated cells of deep convection and to rising air parcels under cyclonic conditions that mix with surrounding air. In the upper troposphere O 3 and CO were found to be correlated with high ΔO 3 /ΔCO ratios of 0.6 to 1.5. In the fold the correlation was strongly negative with ΔO 3 /ΔCO; = −3.5; but the high CO mixing ratios of 100 ppb at O 3 mixing ratios of 250 ppb point to earlier injection of tropospheric air, in agreement with the UFP measurements.