The utilization of lignin from different lignocellulosic biomass is the hot topic for the biorefinery of biomass. In this paper, magnetic lignin nanoparticles (MLN) were prepared by kraft lignin from bamboo residue and Fe3O4 with different ratios via Mannich reaction. The surface morphology and structure of magnetic lignin were characterized and analyzed by X-ray powder diffraction, Fourier transform infrared spectroscopy, and transmission electron microscopy, which confirmed that the MLN were successfully prepared. The performance of MLN adsorbents was evaluated by adsorbing Congo red solution at different initial concentrations and contact times. The results showed that [email protected] (1:0.5) had the best adsorption effect on Congo red solution. When the concentration of Congo red reached 0.6 g/L, [email protected] (1:0.5) had the best adsorption effect on Congo red, reaching 95.5% in only 30 min. As lignin is modified by Fe3O4, it can be recovered by magnetic substances after adsorption and has good reuse performance. The results of adsorption kinetics and adsorption isotherm showed that except for the adsorption process of [email protected] (1:0.5), which is consistent with the chemical adsorption of the multimolecular layer, the adsorption process of other adsorbents is in accordance with the chemical adsorption of the monomolecular layer. In terms of environmental protection and adsorption efficiency, and MLN has become an ideal adsorbent for Congo red dyes due to its simple preparation, superior performance, and convenient recovery.