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The C−H alkylation of aniline derivatives with both primary and secondary alkyl halides was achieved with a versatile nickel catalyst of a vicinal diamine ligand. Step‐economic access to functionalized 2‐pyrimidyl anilines, key structural motifs in anticancer drugs, is thus provided. The C−H functionalization proceeded through facile C−H activation and SET‐type C−X bond cleavage with the assistance of a monodentate directing group, which could be removed in a traceless fashion.