Aerosol particles play a critical role in the tropical tropopause layer (TTL) through cloud formation and heterogeneous chemistry, influencing the radiative and chemical balance of the stratosphere. However, aerosol measurements in the TTL are sparse, resulting in poor knowledge of aerosol abundance and distribution in this important region. Here, we present in situ aircraft measurements over the western tropical Pacific, revealing a persistent and altitude-dependent enhancement of aerosol mass in the TTL compared to the convectively influenced troposphere below. Notably, our data demonstrate a striking positive correlation between aerosol mass and ozone. Model simulations suggest that organic materials constitute a substantial fraction of the total aerosol mass within the TTL. We further derived an empirical parameterization of TTL aerosol mass as a function of ozone. Given the relative ease of ozone measurements and modeling, the parameterization provides a promising framework for estimating TTL aerosol abundance and its effects on climate.