Cellulose nanofibrils (CNFs), disintegrated from natural fibers, are promising alternatives in wastewater purification for the porous structure and numerous hydroxyls. The pristine CNFs aerogel has limited mechanical strength and are vulnerable to collapse when exposed to water. In this work, eco-friendly and recycled CNFs aerogel adsorbents were successfully prepared using cellulose nanofibrils (CNFs), which cross-linked by poly(vinyl alcohol) (PVA) and acrylic acid (AA). The combination of PVA and AA endowed CNFs aerogel strong three-dimensional porous structure and desirable adsorption properties. The heavy metal ions were adsorbed on the CNFs-PVA-AA (CPA) adsorbents efficiently and the maximum adsorption capacities for Cu2+ and Pb2+ approached 30.0 mg/g and 131.5 mg/g, respectively. The CPA adsorbent also showed excellent reusability and their adsorption capacities maintained 89% and 88% for Cu2+ and Pb2+ after 5 repeated uses. The adsorption of these heavy metal ions were confirmed to follow pseudo-second-order kinetic and Langmuir isotherm model. The functions of C ═ O and -OH were the major adsorption sites. Chemical adsorption combined with the porous physical adsorption made the CPA to be excellent adsorbent for the removal of heavy metal ions in wastewater.