Nanocomposites composed of polyacrylamide and nanoclay were synthesized via free-radical cross-linking polymerization and used to adsorb Co2+ and Ni2+ ions from water. The polyacrylamide (PAM)/sodium montmorillonite (Na-MMT) nanocomposites were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, and scanning electron microscopy to confirm the interaction between montmorillonite and the polymer matrix. The effects of pH and heavy metal ion concentration on the adsorption capacity of PAM/Na-MMT were evaluated to determine suitable operating conditions for further experiments. Batch adsorption experimental data were fitted to Langmuir and Freundlich models, which provided information about the adsorption mechanism and the adsorbent surface. The highest Ni2+ removal yield was found to be 99.3% using the 2:1 (w/w) nanocomposite at pH 6 in 100 ppm of Ni2+ solution. The Co2+ removal yield was 98.7% at pH 6 in 60 ppm of Co2+ solution using the 4:1 (w/w) nanocomposite. These results were higher than those obtained by polyacrylamide and nanoclay under the same conditions (removal yield between 87.40 and 94.50%), indicating that PAM/Na-MMT nanocomposites remove heavy metal water pollutants more efficiently and can be used as a novel adsorbent for further industrial applications.