Atrazine (ATZ) adsorption in two natural soils amended with biochars produced from different feedstocks at 300, 500, and 700 °C were investigated; further, the relationships between the surface and partition adsorption capacities of ATZ in biochar-amended soils with biochar characteristics were quantitatively evaluated. The results revealed that high aromaticity, hydrophobicity, and low polarity of biochar facilitated ATZ adsorption. The addition of selected biochars significantly increased the adsorption of ATZ on paddy soil (PS) and black soil (BS) by 5.2–7.5 times and 2.3–4.2 times, respectively. On the contrary, the degree of increase in surface adsorption was much higher than that in partition adsorption, mainly due to the role of the specific adsorption of ATZ on biochar. Meanwhile, the respective contributions of surface and partition adsorptions to the total ATZ adsorption on biochar-amended soil changed with different addition amounts of biochar. The multiple nonlinear regression analysis demonstrated the linear dependence of H/C ratio, (O + N)/C ratio, and specific surface area (SSA) of biochar on the surface adsorption capacity of biochar-amended PS and BS, as well as the linear dependence of organic carbon and ash contents on the partition adsorption capacity of biochar-amended PS and the linear dependence of the H/C ratio and SSA on the partition adsorption capacity of biochar-amended BS. In biochar-amended soil systems, interactions between biochar and soil could affect ATZ adsorption, and organic matter in biochar might compensate for the role of soil organic matter in the competition for adsorption sites with a decrease in the biochar pyrolysis temperature.