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Catalytic dehydrogenative cross‐coupling of two C–H bonds represents a green strategy in view of the atom‐ and step‐economy. However, the challenge is to discover a new innovative bond strategy, especially for the direct coupling between Csp2–H and benzylamines (BzAs). A series of biaryls and bi(hetero)aryls were prepared from commercially available substituted BzAs, AgNO3, cheap K2S2O8 as an oxidant,...