Organic pollutants are widespread and a known problem for the environment. p-nitrophenol (PNP) is one such pollutant found in effluents from various industries involved with pesticides, pharmaceuticals, petrochemicals, plastic, paper, and other materials. The objective of this research was to prepare and test organically modified clays using four different surfactants and to evaluate the removal efficiency of PNP from aqueous solutions. Organically modified clays have attracted great interest due to their wide applications in industry and environmental protection as sorbents for organic pollutants. Two natural smectite-dominated clay types from outcrops in Latvia and Lithuania as well as industrially manufactured montmorillonite (Mt) clay were modified using different nonionic (4-methylmorpholine N-oxide (NMO) and dimethyldodecylamine N-oxide (DDAO)) and cationic (benzyltrimethyl ammonium chloride (BTMAC) and dodecyltrimethyl ammonium chloride (DTAC)) surfactants. Modified clay materials were characterized by Fourier-transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), and the Brunauer-Emmett-Teller method (BET) for surface area analysis. Sorption of PNP was investigated under various conditions, e.g. surfactant loading, initial PNP concentration, contact time, and pH. The novelty of the present study was to prepare innovative organo-sorbents based on manufactured as well as natural clay samples using cationic surfactants and nonconventional nonionic surfactants as modifiers. The sorption data combined with FTIR and XRD supplementary results suggests that nonionic organo-clay (Mt-DDAO_2) is the most effective sorbent and may serve as a low-toxicity immobilizer of pollutants such as phenols.