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N‐Alkyl‐thio glycolipids (TGL) are proposed as fundamental components in the production of synthetic outer membrane vesicles (S‐OMVs). A small but representative library of glycolipids was prepared by thiol‐ene coupling (TEC), using unprotected thiols in acceptable to good yields (63‐96 %). Multilamellar giant vesicles (GVs) of varying sizes were assembled from mixtures of TGL and 1‐palmitoyl‐2‐oleoyl‐...