In this paper, a carbon dot hydrogel composite (CDs-Hy) capable of efficiently removing Pb(II) was prepared by hydrogen bonding self-assembly in combination with carbon dots and a hydrogel. CDs-Hy was characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS), and the effect of the adsorption conditions on the adsorption efficiency of CDs-Hy was studied. The results of the study showed that the incorporation of carbon dots, on the one hand, significantly increased the adsorption capacity of the material. On the other hand, it can increase the stability of hydrogels in aqueous solution. The possible adsorption mechanisms were further verified as ion exchange and coordination. CDs-Hy is a novel adsorbent material capable of removing Pb2+ efficiently, which can be reused several times with high stability.