Global sea to air iodine emissions, along with organic emissions and their oxidation products, have increased tremendously. This work presents a comprehensive analysis of the humidity mediated changes in ageing aerosols comprising iodide and water soluble dicarboxylic acid using aerosol micro-Raman spectroscopy. The studies in the model system, sodium iodide-malonic acid mixed aerosols, unveiled the depletion in iodide. Mechanistic insights gleaned through comparative studies conducted under inert (nitrogen) and oxidative (air) atmospheres reveal the iodide depletion occurs possibly via oxidation to molecular iodine. The reaction involves gaseous components, diffusion of which across the particles will be impacted by the physical state of the particles, such as viscosity, which in turn is intricately linked to ambient humidity levels. To this end, studies on the temporal evolution of the reaction at three distinct RHs covering 30–80% revealed the enhanced progression of the reaction with increasing humidity. Given that geographical locations serving as major sources for atmospheric iodine typically experience high humidity, these reactions could emerge as an additional process controlling iodine speciation in ageing aerosols.