Growing volumes of textile waste and heavy metal pollution of water are emerging environmental challenges. In an attempt to tackle these issues, a non-woven sorbent based on jute fibers was fabricated by recycling the textile waste from the carpet industry. The influence of contact time, concentration, pH and temperature on the sorption of lead and copper ions from aqueous solutions was studied. In order to enhance the sorption capacity of the non-woven material, in situ synthesis of polyaniline (PANI) in the presence of TiO2 nanostructures was performed. The contribution of TiO2 nanoparticles and TiO2 nanotubes to the uniformity of PANI coating and overall sorption behavior was compared. Electrokinetic measurements indicated increased swelling of modified fibers. FTIR and Raman spectroscopy revealed the formation of the emeraldine base form of PANI. FESEM confirmed the creation of the uniform nanocomposite coating over jute fibers. The modification with PANI/TiO2 nanocomposite resulted in a more than 3-fold greater sorption capacity of the material for lead ions, and a 2-fold greater absorption capacity for copper ions independently of applied TiO2 nanostructure. The participation of both TiO2 nanostructures in PANI synthesis resulted in excellent cover of jute fibers, but the form of TiO2 had a negligible effect on metal ion uptake.