An organophilic clay has been obtained via cation exchange reaction between sodium montmorillonite and the hydrochloride salt of 2-(5-(3,5-diaminophenyl)-1,3,4-oxadiazole-2-yl)pyridine, POBD. Thermogravimetric analysis (TGA) showed that thermal decomposition of the organophilic clay starts at about 350°C, which shows that it is quite thermally stable compared with conventional montmorillonite modified with aliphatic long chain surfactants. POBD-modified organoclay almost quantitatively removed the Co(II) ion from aqueous solution at pH = 10.0 (Qt = 3.00 mg g−1, R = 98.2%). A series of polyimide/clay nanocomposite materials (PCNs) consisting of POBD and benzophenone-3,3′,4,4′-tetracarboxylic dianhydride, BTDA were also prepared by an in situ polymerization reaction via thermal imidization. POBD-modified organoclay was used as a surfactant at different concentrations. Intercalation of polymer chains within the organoclay galleries was confirmed by WXRD. Both the glass transition temperature and thermal stability are increased with respect to pristine PI at low clay concentrations. At high clay loadings, the aggregation of organoclay particles results in a decrease in Tg and thermal stability. In the SEM images of PCN 1 and 3%, too many micro cracks are observed in the background, and a flower-shape pattern spreads uniformly over the entire surface. The maximum Co(II) uptake capacity and efficiency were observed at pH 10.0 within a 40-h period for both PI and PCN films. POLYM. COMPOS., 2011. © 2011 Society of Plastics Engineers