Currently, biochar (BC) has shown promising potential in groundwater and surface-water remediation. In this work, husks based biochar (TBC) was prepared and modified with aquatic animal waste (shrimp and crab) to produce shrimp-modified biochar (SBC) and crab-modified biochar (CBC), respectively. The as-prepared BCs (TBC, SBC, and CBC) were characterized by X-ray diffraction, scanning electron microscopy, elemental analysis, Boehm titration, Fourier transform infrared, and X-ray photoelectron spectroscopy. SBC and CBC had more developed nitrogen-containing functional groups than TBC, which indicates that the crude proteins in shrimp and crab have successfully achieved in situ nitrogen doping. Results of batch experiments showed that SBC and CBC had larger groundwater pollutants (2,4-dichlorophenol (2,4-DCP) and Ni(II)) adsorption capacities than TBC. According to batch adsorption experiment and characterization analysis results, the proposed adsorption mechanism of 2,4-DCP includes hydrogen bonding and π-π electron-donor-acceptor interaction, while the mechanism for Ni(II) adsorption are proposed to be surface complexation, ion exchange, and electrostatic attraction.