Waste emissions have increased the amount of water and soil contaminated with heavy metals such as Pb. To broaden the methods for the recycling and environmental usage of cow manure (CM) and its vermicompost (CV), CM, CV, and their derived biochars produced by the pyrolysis of CM or CV at 350 and 700 °C were used as adsorbents for Pb2+ removal in this batch adsorption experiment to reveal their different Pb2+ removal efficiencies and the underlying mechanisms. The batch experiment results revealed that all adsorbents rapidly removed Pb2+ within 30 min. A pH between 2.0 and 6.0 positively affected Pb2+ removal by CM and its biochar, whereas that by CV and its biochar was only positively affected by pH between 2.0 and 3.0. CV-derived biochar was more effective in the removal of Pb2+ than the other absorbents, with the maximum adsorption capacities (Qm) fitted from the Langmuir model reaching approximately 230.0 mg·g−1 and the desorption rate (DR) being approximately 0.00–0.02%. Material physiochemical characterization, including X-ray diffraction analysis, showed that high pH, high ash content, rich mineral content, and high mineral contents might have been the main reasons for more effective removal of Pb2+ from aqueous solutions by CV-derived biochar. Fourier-transform infrared analysis indicated that surface functional groups such as –OH, C O, –COO–, and C–O; original and newly produced carbonate; and phosphate in CV also led to more effective Pb2+ removal efficiency from aqueous solution via surface functional group binding. Thus, pyrolyzing CVs may be used to produce biochar as a cost-effective adsorbent for heavy metal remediation in soil and water in the future.