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Aerosol particles in the atmosphere have the ability to uptake water and form droplets. The droplets formed can interact with solar radiation (indirect effect of aerosols) and influence the net radiative forcing. However, the magnitude of change in radiative forcing due to the indirect effect of aerosols remains uncertain due to the high variance in aerosol composition and mixing states, both spatial and temporally. As such, there is a need to measure the water-uptake of different aerosol particle groups under controlled conditions to gain insight into the water-uptake of complex ambient systems. In this work, the water-uptake (hygroscopicity) of internally and externally mixed ammonium sulfate – organic binary mixtures were directly measured via three methods and compared to droplet growth prediction models. We found that subsaturated water-uptake of ammonium sulfate-organic mixtures agreed with their supersaturated hygroscopicity, and mixing state information was able to be retrieved at both humidity regimes. In addition, we found that solubility-adjusted models may not be able to capture the water-uptake of viscous particles, and for soluble organic aerosol particles, bulk solubility may not be comparable to their solubility in a droplet. This work highlights the importance of using multiple complementary water-uptake measurement instruments to get a clearer picture of mixed aerosol particle hygroscopicity, especially for increasingly complex systems.