This study reports the synthesis of a polyaniline@waste tissue paper (PANI@WTP) nanocomposite via in situ oxidative polymerization for removing Cu(II) and phenol from wastewater. The nanocomposite achieved maximum Langmuir adsorption capacities of 605.20 mg/g for Cu(II) and 501.23 mg/g for phenol, outperforming many conventional adsorbents. The material was regenerable over five cycles and showed practical utility in synthetic tap and groundwater matrices.