In this study, Na-montmorillonite was organically modified with cetyltrimethylammoniumbromide (CTAB) and intercalated with in-situ polymerized indene. Polyindene(PIn)/Organo-MMT nanocomposites were obtained with three different compositions and coded as: K1: [PIn(94.5%)/O-MMT(5.5%)], K2: [PIn(92.8%)/ O-MMT(7.2%)], and K3: [PIn(87.9%)/O-MMT(12.1%)].These nanocomposites were subjected to full characterization with various techniques. Electrokinetic studies were conducted to reveal the zeta (f)-potential characteristics of the nanocomposites. f-potentials of the materials were observed to decrease with increasing O-MMT content. The cationic (CTAB) and anionic (sodium dodecylsulfate) surfactants were shifted the f-potentials of the colloidal dispersions to more positive and more negative regions, respectively whereas nonionic surfactant (Triton X-100) caused almost no change. The pH and temperature were observed to shift the f-potential values of the nanocomposites to more negative and slightly more positive regions, respectively. With the addition of mono (NaCl), di (BaCl 2 ) and three (AlCl 3 ) valent salts, the f-potential of the nanocomposites were shifted to more negative, more positive, and much more positive regions, respectively.