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Materials with two-dimensional, geometrically frustrated, spin-1/2 lattices provide a fertile playground for the study of intriguing magnetic phenomena such as quantum spin liquid (QSL) behavior, but their preparation has been a challenge. In particular, the long-sought, exotic spin-1/2 star structure has not been experimentally realized to date. Here we report the synthesis of [(CH3)2(NH2)]3[CuII3(μ3-OH)(μ3-SO4)(μ3-SO4)3]·0.24H2O with an S = 1/2 star lattice. On the basis of the magnetic susceptibility and heat capacity mea