A recipe for facile preparation of high-performance low-temperature magnetic refrigerants based on gadolinium-hydroxy-chloride (GHC), which exhibits a large magnetic entropy change of up to 61.8 J kg À1 K À1 or 318.9 mJ cm À3 K À1 , high thermal stability, strong alkali-resistance and good thermal conductivity, is reported.Cryogenic magnetic cooling, as an environmentally friendly and energy-efficient cooling technique, has received much attention due to its possibility of replacing refrigeration systems involving 3 He, which is in short supply worldwide, to achieve ultra-low temperatures (r4 K). 1 The refrigeration effect is expected for materials with a large magnetocaloric effect (MCE), which is inherently related to a change in magnetic entropy (DS m ) at low temperatures following adiabatic demagnetization. 2 Gadolinium(III) with weak magnetic exchange is an ideal constituent element for magnetic refrigerant materials, because its 8 S 7/2 ground state provides a large magnetic entropy change based on the equation ÀDS m = nR ln(2S + 1)/M w , where the prefix n is the number of uncoupled spins, R is molar gas constant, S is ground state spin of the magnetic center and M w is the formula weight of the compound. In order to obtain novel high performance magnetic coolants, it is necessary to select a light and multidentate ligand to achieve lower M w /N Gd ratios because ÀDS m is inversely-proportional to the molecular weight. 3 Thus, inorganic counterions with a large charge/weight ratio, such as gallates, phosphates, sulfates, carbonates and halides, may be ideal to design dense magnetic coolants. 2,4 For example, gadolinium gallium garnet Gd 3 Ga 5 O 12 (GGG) and its iron-doped compound Gd 3 (Ga 1Àx Fe x ) 5 O 12 (GGIG) are well-known commercially-employed low-temperature magnetic refrigerant materials. 5 Recently, the known compounds Gd(OH)CO 3 6 , GdPO 4 , 7 GdF 3 8 as well as two new compounds based on the sulfate family, Gd 4 (SO 4 ) 4 (OH) 4 (H 2 O) 4 9