The nanocomposites based on organic–inorganic hybrid have been attracting much attention due to their potential applications used as new type of functional materials, such as colloidal stabilizers, electro-optical devices, and nanocomposites materials. The organic–inorganic hybrid of poly(acrylic acid-acrylonitrile)/attapulgite, P(A-N)/AT nanocomposites, were prepared by using in situ polymerization and composition of acrylic acid (AA) and acrylonitrile (AN) onto modified attapulgite (AT) nanoparticles. The resulting P(A-N)/AT nanocomposites were transformed into novel nano-adsorbent of poly(acrylic acid-acryloamidoxime)/attapulgite by further functionalization, i.e. P(A-O)/AT nano-adsorbent. The adsorption properties of P(A-O)/AT toward metal ions were determined, and the results indicated that the adsorbents with nanocomposite structure held a good of selectivity to Pb 2+ among numerous metal ions. The maximum removal capacity of Pb 2+ was up to 109.9mg/g and it is notable to see that the adsorption removal of P(A-O)/AT nano-adsorbent for Pb 2+ could achieve more than 96.6% when the initial concentration of Pb 2+ was 120.0mg/l. The kinetics, isotherm models, and conductivity were introduced to study the adsorption mechanism of P(A-O)/AT for Pb 2+ and it was concluded that it could be chemisorptions process and the best coordination form took place when AO:AA:Pb 2+ =1:1:1. In addition, after simply treated with CTAB, P(A-O)/AT nano-adsorbent showed better adsorption properties for phenol than the same kinds of materials.