A process for producing a particulate composition comprising crystalline α,α-trehalose dihydrate with an α,α-trehalose content of 98.0% by weight or more, on a dry solid basis, and a degree of crystallinity for crystalline α,α-trehalose dihydrate of 90.0% or higher, when calculated based on its powder X-ray diffraction profile, said process comprising the steps of: obtaining a saccharide solution with an α,α-trehalose content of over 86.0% by weight, on a dry solid basis, without passing through a fractionation step by column chromatography, by allowing to act on liquefied starch an α-glycosyltrehalose-forming enzyme derived from a microorganism of the genus Arthrobacter and a trehalose-releasing enzyme derived from a microorganism of the genus Arthrobacter along with a starch debranching enzyme and a cyclomaltodextrin glucanotransferase, followed by allowing a glucoamylase to act on the resulting mixture; precipitating crystalline α,α-trehalose dihydrate from said saccharide solution; collecting the precipitated crystalline α,α-trehalose dihydrate by a centrifuge; and ageing and drying the collected crystals; wherein said cyclomaltodextrin glucanotransferase is a natural or recombinant cyclomaltodextrin glucanotransferase derived from a microorganism of the species Paenibacillus illinoisensis, Paenibacillus pabuli, or Paenibacillus amylolyticus, or an enzyme having the amino acid sequence of SEQ ID NO: 12 or 13; wherein said step of precipitating crystalline α,α-trehalose dihydrate is conducted by a controlled cooling method or semi-controlled cooling method; and wherein said controlled cooling method is a cooling method where the liquid temperature "T" at the time "t" is expressed by the following formula "T=T 0 -(T 0 -T f) (t/ τ) 3 ", wherein " τ " is the operation time established for a crystallization step, "T 0 " is the liquid temperature at the initiation of crystallization, and "T f " is the targeted liquid temperature at the termination of crystallization. obtaining a saccharide solution with an α,α-trehalose content of over 86.0% by weight, on a dry solid basis, without passing through a fractionation step by column chromatography, by allowing to act on liquefied starch an α-glycosyltrehalose-forming enzyme derived from a microorganism of the genus Arthrobacter and a trehalose-releasing enzyme derived from a microorganism of the genus Arthrobacter along with a starch debranching enzyme and a cyclomaltodextrin glucanotransferase, followed by allowing a glucoamylase to act on the resulting mixture; precipitating crystalline α,α-trehalose dihydrate from said saccharide solution; collecting the precipitated crystalline α,α-trehalose dihydrate by a centrifuge; and ageing and drying the collected crystals; wherein said cyclomaltodextrin glucanotransferase is a natural or recombinant cyclomaltodextrin glucanotransferase derived from a microorganism of the species Paenibacillus illinoisensis, Paenibacillus pabuli, or Paenibacillus amylolyticus, or an enzyme having the amino acid sequence of SEQ ID NO: 12 or 13; wherein said step of precipitating crystalline α,α-trehalose dihydrate is conducted by a controlled cooling method or semi-controlled cooling method; and wherein said controlled cooling method is a cooling method where the liquid temperature "T" at the time "t" is expressed by the following formula "T=T 0 -(T 0 -T f) (t/ τ) 3 ", wherein " τ " is the operation time established for a crystallization step, "T 0 " is the liquid temperature at the initiation of crystallization, and "T f " is the targeted liquid temperature at the termination of crystallization.