Batch and leaching experiments were conducted to investigate the adsorption and removal of Escherichia Coli (E. coli) from water by crop straw biochars and Al(III)-modified biochars. Results indicated that the amount of E. coli adsorbed by non-modified crop straw biochars was very low, while Al(III)-modified crop straw biochars showed great adsorption capacity and high removal efficiency for E. coli. The adsorption capacity of the biochars modified by 0.6 mol/L Al(III) was greater than that of the biochars modified by 0.3 mol/L Al(III). When the concentration of E. coli was less than 0.63 mg/ml, the removal percentage ofE. coli was 100% by Al(III)-modified soybean straw biochar and more than 96% and 90% by Al(III)-modified peanut straw bioachar and Al(III)-modified rice straw biochar, respectively. In leaching experiment, when the suspension of 0.63 mg/ml E. coli passed through the leaching column containing 2 g Al(III)-modified rice straw biochar, 152 leachates were continuously collected with each leachate of 10 ml. The concentration of E. coli in most leachates was less than 0.02 mg/ml and the removal percentage of E. coli from the suspension was above 95%. Therefore, Al(III)-modified crop straw biochars can be used to remove E. coli from water efficiently.