Abstract: This paper reports on a molecular dynamics investigation of the molecular organization of alkanethiolates (from ethane to dodecanethiolate) on octahedral and cubic gold nanocrystals with diameters up to 10 nm. We show that the average surface per adsorbed thiolate only slightly depends on the nanocrystal shape and the alkane chain length. Two different organizations of thiolates are observed on the facet centers and edges of octahedral nanocrystals, while on cubic nanocrystals only one appears...