A method for producing high purity D-psicose crystals having a purity of 98% (w/w) or more and a grain size of MA200 or more. The method includes: removing impurities from a D-psicose solution to obtain a purified D-psicose solution； concentrating the purified D-psicose solution； cooling the concentrated D-psicose solution to 30°C to 40°C through a heat exchanger； seed crystallizing the D-psicose solution at 30°C to 40°C to obtain a seed crystallized massecuite； and full-scale crystallizing the seed crystallized massecuite. The method can produce pure D-psicose crystals in a suitable form for industrial application through an economical crystallization process from the D-psicose solution without using organic solvents.
