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Carboranes, a class of stable icosahedral boron–carbon molecular clusters with 3D aromaticity, exhibit broad applications in materials chemistry, organic synthesis, and pharmaceutical science. Accordingly, the selective functionalization of carboranes has garnered significant research interest. In this work, a novel Pd‐catalyzed direct B–H/C–H coupling between carboranes and a broad range of (hetero)arenes is reported. This method features excellent B(9)‐site selectivity for o ‐ and m ‐carboranes, along with high reactivity toward simple arenes, five‐membered heterocycles, and benzofused five‐membered heterocycles, all without the need for any directing groups. More details are discussed in the article by Sun et al . on pages 786—794. image