Sea spray aerosol (SSA) represents the largest source of natural primary aerosol with climate relevance in cloud formation. The aerosol-cloud activation process is influenced by saccharides, which comprise a large SSA organic mass fraction. Saccharides are enriched relative to sodium in SSA by several orders of magnitude but the mechanisms of that enrichment remain poorly understood. Here, saccharide enrichment in laboratory-generated SSA was quantified via bubble bursting experiments using marine-relevant model systems. The resulting particles exhibited core−shell morphology previously observed in SSA, as identified by single particle atomic force microscopy (AFM). Measured enrichment factors (EFs) from filters indicated significant enrichment in aerosol <250 nm in diameter (EF = 1.68 ± 0.19) for the anionic polysaccharide (alginate) and no enrichment (EF = 1) for neutral short-chain saccharides (glucose, sucrose, raffinose, and cyclodextrin). Concurrent surface tension depression was observed for the surface microlayer (SML) with alginate (−Δ12.2 mN m −1 relative to seawater matrix) but not for the short-chain saccharides. Together, results indicate that surface activity of these systems result in saccharide enrichment. Moreover, model system complexity was increased through calcium addition which significantly increased alginate enrichment in aerosol <250 nm in diameter (EF = 2.44 ± 0.26). Separately, protein addition caused the greatest alginate enrichment increase in 500−1000 nm diameter aerosol (EF = 5.77 ± 0.61). These results indicate saccharide surface activity and cooperative interactions with protein and calcium that enhance saccharide enrichment. However, the model systems have not reproduced EFs of natural SSAs and the role of complex ocean biology still needs to be evaluated.