This study is focused on determining the type and quantity of REE impurities responsible for converting the structure of NdSc3(BO3)4 into an R32 polymorph. According to the single crystal X-ray diffraction of RxNdyScz(BO3)4 (R = Sm–Lu, x + y + z = 4) the samples probably contain several polymorphic modifications. However, the predominant structure has been defined as R32 for R = Eu, Er, Tm, and Yb and P3221 for R = Sm, Gd, Tb, Dy, and Ho. Another potential limitation to the future use of the crystals is a compositional zoning found in the crystals with significant substitution in the scandium position. [ABSTRACT FROM AUTHOR]