Atmospheric deposition is an important source of the micronutrient selenium for terrestrial ecosystems and food chains. However, the factors determining the total concentrations and chemical forms (speciation) of selenium in atmospheric deposition remain poorly understood. Here, aerosol samples were collected weekly over 5 years at Pic du Midi Observatory (French Pyrenees), alongside highly temporally resolved samples of aerosols, precipitation, and cloud water taken during a 2-month campaign. Firstly, measurements of selenium, other elements, and water isotopes were combined with sophisticated modelling approaches (aerosol-chemistryclimate SOCOL-AERv2 model and air parcel backward trajectories and Lagrangian moisture source analyses). Aerosol selenium measurements agreed well with SOCOL-AERv2-predicted values, and interestingly, higher fluxes of selenium and other elements were associated with deep convective activity during thunderstorms, highlighting the importance of local cloud dynamics in high deposition fluxes. Our results further indicate the coupling of element and water cycles from source to cloud formation, with decoupling during precipitation due to below-cloud scavenging. Secondly, selenium speciation was investigated in relation to sulfur speciation, organic composition, and moisture sources. While in the 5-year aerosol series, selenite (Se IV ) was linked to anthropogenic source factors, in wet deposition it was related to pH and Atlantic moisture sources. We also report an organic selenium fraction, tracing it back to a marine biogenic source in both aerosols and wet deposition. With a comprehensive set of observations and model diagnostics, our study underscores the role of weather system dynamics alongside source contributions in explaining the atmospheric supply of trace elements to surface environments.