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The rare-earth tetraborides are exceptional in that the rare-earth ions are topologically equivalent to the frustrated Shastry-Sutherland lattice. In this paper, we report the growth of large single crystals of <i>R</i>B<inline-formula> <math display="inline"> <semantics> <msub> <mrow></mrow> <mn>4</mn> </msub> </semantics> </math> </inline-formula> (where <i>R</i> = Nd, Gd &#8594; Tm, and Y) by the floating-zone method, using a high-power xenon arc-lamp furnace. The crystal boules have been characterized and tested for their quality using X-ray diffraction techniques and temperature- and field-dependent magnetization and AC resistivity measurements.