The goal of the present paper is to explore the properties of medium molecular-weight chitosan/polyvinyl alcohol blends mixed in volume ratios of 75:25, 50:50, and 25:75 obtained by solution casting. Cross-linked chitosan/poly(vinyl alcohol) nanostructures were obtained by treating these blends with 5% (v/v) glutaraldehyde. The prepared chitosan/polyvinyl alcohol films were characterized by attenuated total reflectance - Fourier transform infrared spectroscopy (FT-IR), dynamic light scattering, and cytotoxicity, while the nanostructured materials were examined by scanning electron microscopy, differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), and X-ray diffraction. Also, the removal of lead(II) ions from aqueous solution by adsorbents nanostructures was studied in the batch adsorption mode. The effects of adsorbent dosages, initial metal concentration, and contact time on the adsorption capacity were investigated. The FT-IR spectra indicated the interactions of polyvinyl alcohol with chitosan. DSC and TGA analyses revealed the loss of water up to 100 °C. The zeta potential and mobility of the prepared nanostructures were enhanced with the increasing ratio of the cationic polymer. The results showed that the 100% chitosan adsorbent provided the highest removal of Pb(II) during the first 15 min (̴94%). The chitosan100/polyvinyl alcohol0 and chitosan75/polyvinyl alcohol25 nanostructures fitted well with the Langmuir isotherm model. The maximum adsorption capacities for Pb(II) ions reached maxima of 7.36 and 7.67 mg/g, respectively. The Freundlich isotherm model best described the Pb(II) adsorption on the 50% chitosan/50% polyvinyl alcohol and 25% chitosan/75% polyvinyl alcohol adsorbents. Furthermore, (3-(4,5-dimethylthiazol-2-yl)-2,5- diphenyltetrazolium bromide (MTT) assay results demonstrated that chitosan/polyvinyl alcohol films are biocompatible with more than 90% cell viability.