Dodecylbenzenesulfonate (DBS) modified NiRTi layered double hydroxides (LDHs) with different Ni/Ti molar ratios were prepared as hydrophobic organics sorbent by one-step co-precipitation method. The basal spacing of DBS-NiRTi (d(003) = 2.99-3.54 nm) is significantly increased compared with cyanate-intecalated NiSTi-LDH (0.73 nm) due to the intercalation of surfactant anions between the LDH layers. The greatly enhanced contact angle (123.5-144.2 degrees) for water and the reduced surface area (1.72-3.25 m(2)/g) of DBS-NiRTi nanocomposites demonstrate their strong hydrophobic property. The highest sorption capacity for pentachlorophenol (PCP) of DBS-NiSTi among all samples is intimately related to its stacking model of the interlayer hydrophobic moiety and organic carbon content. The linear model well-fits for PCP sorption isotherms on DBS-NiRTi (R-2 > 0.96), implying a partitioning sorption process. Along with the effect of medium pH and temperature on PCP sorption-desorption study on DBS-NiSTi, an adsolubilization mechanism, an exothermic sorption nature, and a significant hysteresis phenomenon during sorption-desorption process are revealed.