AbstractMarine cloud brightening (MCB) has been proposed as a viable way to counteract global warming by artificially increasing the albedo and lifetime of clouds via deliberate seeding of aerosol particles. Stratocumulus decks, which cover wide swaths of Earth’s surface, are considered the primary target for this geoengineering approach. The macroscale properties of this cloud type exhibit a high sensitivity to cloud microphysics, exposing the potential for undesired changes in cloud optical properties in response to MCB. In this study, we apply a highly detailed Lagrangian cloud model, coupled to an idealized parcel model as well as a full three-dimensional large-eddy simulation model, to show that the choice of seeded particle size distribution is crucial to the success of MCB, and that its efficacy can be significantly reduced by undesirable microphysical processes. The presence of even a small number of large particles in the seeded size spectrum may trigger significant precipitation, which will reduce cloud water and may even break up the cloud deck, reducing the scene albedo and hence counteracting MCB. On the other hand, a seeded spectrum comprising a large number of small particles reduces the fraction of activated cloud droplets and increases entrainment and evaporation of cloud water, which also reduces the efficiency of MCB. In between, there may exist an aerosol size distribution that minimizes undesirable microphysical processes and enables optimal MCB. This optimal size distribution is expected to be case dependent.