Organopalygorskites were synthesised by using dimethyldioctadecylammonium bromide (DMDOA) and cetylpyridinium chloride (CP) with surfactant loadings equivalent to 100% and 200% CEC of the palygorskite. The four organopalygorskites, thus produced, were characterised by Fourier Transform Infrared Spectroscopy (FTIR), thermogravimetric analysis (TGA), scanning electron microscopy (SEM) and zeta potential measurement. FTIR and TGA data demonstrated that higher surfactant loadings as well as long branched chain DMDOA produced highly ordered surfactant conformation. SEM morphological results showed that the organopalygorskites had less entangled fibres than the unmodified palygorskite. The zeta potential values showed positive charge formation on the organopalygorskites surface when they were synthesised with surfactant loadings equivalent to 200% CEC of the palygorskite. The organopalygorskites were tested for adsorption of p-nitrophenol (PNP) with a special focus on the adsorption isotherms. The adsorption data could be fitted with multiple isothermal models indicating that the adsorption was controlled by multiple mechanisms. Sorbent loading rate, initial pH, temperature and ionic strength might all affect the adsorption process. Also, DMDOA modified organopalygorskites reduced desorption/redispersal of adsorbed PNP back into the environment to a great extent. This study will be helpful in designing palygorskite-based organoclay adsorbents for remediating organic environmental contaminants which are ionic in nature.