Chitosan modification is an important method for the development of adsorbents that has attracted considerable interest in recent years. In this regard, a new type of efficient Pb(II) adsorbent was prepared in a simple and cost-effective way. In this study, carboxylated chitosan (CYCS) and carboxylated nanocellulose (CNC) were used to chelate and synthesize hydrogel spheres with effective adsorption sites, in calcium chloride solution. The prepared carboxylated chitosan/carboxylated nanocellulose (CYCS/CNC) hydrogel beads were used as Pb(II) adsorbents, and using scanning electron microscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy, the structure and adsorption properties of the prepared beads were investigated. The CYCS/CNC adsorbents exhibited an excellent aqueous Pb(II) adsorption capacity (qm = 334.92 mg g−1), and the experimental results further revealed that the adsorption data fitted well with the Langmuir model, and the adsorption kinetics accorded with the pseudo-second-order model. Additionally, the adsorption mechanism was identified as monolayer chemisorption.