Contamination of water resources by toxic heavy metals has significant impacts on environmental and human health. Their removal from aqueous media is essential to ensure water sustainability and to provide safe freshwater availability to population. Electrospun chitosan (CS) nonwoven mats are efficient at removing heavy metals from aqueous media. However, they suffer from low permeability and low-mechanical strength. They are also unable to remove contaminants in a nonselective way. A bilayer sorbent media made of a porous phosphorylated cellulose substrate covered by electrospun CS nanofibers was developed to overcome those weaknesses. The hydrophilic composite shows good water permeability and mechanical strength with appropriate thermal and chemical characteristics. Adsorption tests with Cd(II) indicate that pseudo-second order and Langmuir models best fitted experimental data, with a maximum adsorption capacity of 591 mg/g at 25 C. Adsorption with multielement samples containing Cr(VI), Cu(II), Cd(II), and Pb(II) also reveal their capability to remove them in a selective way. This mechanically resistant, hydrophilic, and permeable adsorbent media was able to capture both cationic and anionic metallic contaminants.