Bent-core (“banana–shaped”) molecules exhibit chiral anti-ferroelectric mesophases, which are promising for a range of applications including light shutters and memory devices. This liquid crystal alignment can be directed by self-assembly at a water surface. To illuminate the self assembly process, molecular dynamics simulations are carried out on systems of composed of 4,6-dichloro-1,3- phenylene bis[4-(4-n-subst.-phenyliminomethyl)benzoates] molecules adsorbed on water surfaces. The simulation results elucidate both the intra-molecular and inter-molecular structure and dynamics associated with the self-assembly.