A novel compound barrier technology for the control of phosphorus and nitrogen release from sediments was reported. The compound barrier was constructed with zeolite and calcite. Using this compound barrier technology, various influencing factors of phosphorus release from the sediments were investigated. The results showed that the compound barrier with calcite and zeolite can not only control the ammonia release from the sediment, but also reduce the phosphorus release from the sediment effectively. The efficiency of the compound barrier to immobilize the phosphorus of sediments increased with the increment of the quantity of zeolite or calcite. The efficiency was also affected by the grain size of the zeolite. The less the grain sizes of the zeolite, the more the efficiency. The construction mode of the compound barrier played an important role in the control efficiency of phosphorus release from the sediments. It was found that the efficiency of barrier mixed with zeolite and calcite was slightly less than that of the barrier made up of zeolite (underlayer) and calcite (superstratum). The compound barrier with zeolite (underlayer) and calcite (superstratum) can control phosphorus release much more efficiently than the barrier with zeolite (superstratum) and calcite (underlayer).