Organo-fluorohectorites were either obtained commercially or synthesized by reacting unmodified fluorohectorite with ammonium salts. Modified and unmodified fluorohectorites were incorporated into low density polyethylene (LDPE) with or without maleic anhydride grafted polyethylene (MAPE) as a compatibilizer. Although clay aggregates were observed for all blends, the existence of an intercalated and exfoliated clay structure was confirmed according to morphological observations. Different types of cationic organomodifier were comparatively studied. It was found that alkyl chain length and amount of organomodifier were two factors influencing the dispersion state of fluorohectorites. Nanocomposites containing well-dispersed fluorohectorites showed superior mechanical and barrier properties as compared to their counterparts. The presence of MAPE exhibited beneficial effects on the mechanical properties of the fluorohectorite/LDPE system, whereas the water vapour barrier property was adversely affected.