Abstract: A nickel-catalyzed three-component carbonylative cross-coupling reaction of allylic alcohols and organoalanes with CO at atmospheric pressure is reported, enabling the expedient formation of b,g-unsaturated ketones with broad scope. Particularly, the chemoselective allylic carbonylation of dios further highlights the practicability of this protocol. The leverage of organoalanes as both the coupling components and the activators for the alcohol functionalization is crucial for this method, thus no extraneous activators are required.