Hexavalent chromium in aqueous solutions was successfully removed via sorption and reduction in the presence of waste leaves. Cr(VI) removal followed a first-order reaction, and removal rates were proportional to the amount of waste leaves used in the tests. Most of Cr(VI) were removed via sorption in early stages of the tests, but the reduction reaction played a significant role in Cr(VI) removal later. Solution pHs were continuously decreased due to the microbial activity, which was induced from the microorganisms attached on waste leaves. The decreased solution pHs further enhanced the sorption and reduction of Cr(VI). To characterize the microorganisms found in the tests, a denaturing gradient gel electrophoresis (DGGE) method was used. The majority of microorganisms were composed of Bacillus sp. which can reduce Cr(VI). Thus, waste leaves can be effective reactive media for the treatment of Cr(VI) in the subsurface.