Atmospheric aerosols can exist as supersaturated (metastable) liquid or glassy states, with physical and chemical properties that are distinct from the solid or liquid phases. These unique properties of aerosols have substantial implications on climate and health effects. Direct investigations on metastable aerosols remain a challenge because any interfacial contact can cause heterogeneous nucleation. In this study, in situ Raman spectroscopic and Mie scattering imaging analysis is applied to metastable aerosols in the absence of physical contact using an environment-controlled electrodynamic balance (EDB). This has allowed a detailed study of the O-H stretching regions of the Raman spectrum, revealing evidence for the rearrangement of hydrogen-bonding structures of levitated aqueous citric acid (CA) and aqueous sucrose droplets at metastable liquid states. We found that carboxyl groups in a CA droplet yield distinctive dynamics of strong and weak hydrogen bonds, whereas hydroxyl groups in a sucrose droplet show correlated strong and weak interactions. Such effects are particularly important in a supersaturated solution. These results indicate that metastable liquid aerosols from different sources may exhibit distinct physical and chemical behavior.