Hooking up: FeCl(2) catalyzes the efficient cross dehydrogenative arylation of substrates having benzylic C-H bonds (see scheme). High regioselectivity was observed during the cross-coupling between compounds containing aromatic C(sp(2))-H bonds and benzylic C(sp(3))-H bonds. This process is proposed to proceed by single-electron-transfer oxidation and Friedel-Crafts alkylation.