A simple method for synthesizing highly wrinkled and less layered structure of graphene sheets by using a mechano-thermal exfoliation method was developed. During this process, graphite and ammonium chloride(NH_4Cl) powders were loaded by milling and followed with heating at a quartz tube under a nitrogen gas flow. The method is facile and easy for scaling up. Consequently, such microstructure merits of structure endowed graphene super strong adsorption ability, which should have great potential for water purification and treatment. A simple method for synthesizing highly wrinkled and less layered structure of graphene sheets by using a mechano-thermal exfoliation method was developed. During this process, graphite and ammonium chloride (NH 4 Cl) powders were loaded by milling and followed with heating at a quartz tube under This method is facile and easy for scaling up. Therefore, such microstructure merits of structure endowed graphene super strong adsorption ability, which should have great potential for water purification and treatment.