Surface properties of atmospheric aerosol particles are crucial for accurate assessments of the fates of liquid particles in the atmosphere. Surface tension directly influences predictions of particle activation to clouds, as well as indirectly acting as a proxy for chemical surface partitioning. Challenges to accounting for surface effects arise from surface tension dependence on solution concentration and the presence of complex aqueous mixtures in aerosols, including both surface-active organic solutes and inorganic electrolytes. Also, the interface itself is varied, in that it may be a liquid-vapor interface, as in the surface of an aerosol particle with ambient air, or a liquid-liquid interface between two, immiscible liquids, as in the interior surfaces that exist in multiphase particles. In this Feature Article, we highlight our previous work entailing thermodynamic modeling of liquid-vapor surfaces to predict surface tension and microscopic examinations of liquid-liquid interfacial phenomena to measure interfacial tension using biphasic microscale flows. New results are presented for binary aqueous organic acids and their ternary solutions with ammonium sulfate. Ultimately, improved understanding of aerosol particle surfaces would enhance treatment of aerosol particle-to-cloud activation states and aerosol effects on climate.