A new process is proposed to prepare high-quality syngas (H-2 + CO) for the production of dimethyl ether, methanol, and other chemical products at atmospheric pressure, during which the pulverized coal is used as raw material. The process consists of two zones: reduction and oxidation. Steam is injected into the reduction zone, which then reacts endothermically with coke to produce syngas. The raw material (pulverized coal) is fed to the oxidation zone and then reacts with air and releases heat. Circulating coal ash and char are heated in the oxidation zone, which provide heat for the reduction zone to maintain the endothermic reactions. The coke just reacts with the steam in the reduction zone, and the gas composition mainly contains H-2 and CO. Therefore, high-quality syngas is produced. To acquire the operating parameters and provide reference for the industrial design, the feasibility of the proposed cycle was verified by preliminary experiments and a system model was built with Aspen Plus to simulate the process. The simulation study shows that the main components of syngas (H-2 + CO) in the new process account for over 85%, reaching up to 93.20%; the ratio of H-2/CO is adjustable between 1.0 and 2.0, which meets the requirement of the production for downstream chemical products. In addition, pilot experiments were carried out based on the model. As a result, the simulation results agree with the experimental data under the same operation condition in three different cases.