More than 20 countries are still suffering problems of excessive fluoride containing water, and greater than 8 mg/L fluoride groundwater has been reported in some villages in China. In order to meet the challenge in the drinking water defluoridation engineering, a high efficiency and affinity defluoridation adsorbent PPy/TiO2 composite was designed and synthetized by in-situ chemical oxidative polymerization. Fourier Transform Infrared Spectroscopy (FTIR), X-ray diffraction Investigator (XRD), X-ray photoelectron spectroscopy (XPS), Thermogravimetric analysis (TG), N-2 isotherm analysis, Scanning Electron Microscopy (SEM) and Zeta potential analysis were conducted to characterize surface and textural properties of the as-prepared PPy/TiO2, and the possibility of fluoride adsorption was carefully estimated by adsorption isotherm and kinetic studies. Characterization investigations demonstrate the uniqueness of surface and textural properties, such as suitable specific surface area and abundant positively charged nitrogen atoms (N+), which indicate the composite is a suitable material for the fluoride adsorption. Adsorption isotherms and kinetics follow better with Langmuir and pseudo-second-order model, respectively. The maximum adsorption capacity reaches 33.178 mg/g at 25 degrees C according to Langmuir model, and particular interest was the ability to reduce the concentration of fluoride from 11.678 mg/L to 1.5 mg/L for drinking water at pH of 7 within 30 min. Moreover, the adsorbent can be easily recycled without the loss of adsorption capacity after six cycles, greatly highlighting its outstanding affinity to fluoride, low-cost and novel to be used in the purification of fluoride containing water for drinking. Furthermore, the adsorption mechanism was extensively investigated and discussed by FTIR investigation and batch adsorption studies including effect of pH, surface potential and thermodynamics. The adsorption is confirmed to be a spontaneous and exothermic process with decreasing entropy, which is prominently conducted through electrostatic attraction, and ionic exchange, and chelation may be also involved. Hydroxyls and positively charged nitrogen atoms play important roles in the adsorption. (C) 2017 Elsevier Inc. All rights reserved.