The removal of NO 3 − from water was performed and compared among four organo-montmorillonites (OMt) with quaternary amine surfactants of different chain lengths [octadecyl trimethyl-(ODTMA), hexadecyl trimethyl-(HDTMA), tetradecyl trimethyl-(TDTMA) and dodecyl trimethyl-ammonium (DDTMA)] and loadings [100%, 200%, 400% of the Mt cation exchange capacity (CEC)]. The maximum adsorption of NO 3 − was attained by the long chain length surfactants (64 and 100 mg NO 3 − ions per gram of OMt, for HDTMA and ODTMA, respectively) with initial loading of 400% with respect to the CEC of Mt. The short chain length surfactants (DDTMA and TDTMA) did not show adsorption of NO 3 − except for TDTMA 400 sample. The NO 3 − adsorption produced a slight expansion of the interlayer thickness of the OMt samples loaded with long-chain surfactants that was assigned to the entrance of NO 3 − by a synergic effect with these surfactants. The decrease of the negative zeta potential, found for OMt samples relative to that of Mt sample, was attributed to the surfactant chain length rather than to the actual surfactant loaded amounts, which allowed attaining positive zeta potential values for the OMt loaded with long-chain surfactants. The NO 3 − adsorption on OMt samples caused a slight decrease in the positive zeta potential values, reflecting the external surface coating by NO 3 −. For long-chain molecules, this behaviour also indicated the formation of greater interactions such as ion pairs between the positive polar group of the surfactant and NO 3 − ions.