A cobalt−diphosphine catalyst has been found to promote a selective 1:2 coupling reaction between aldehydes and allenes to form β,δ-dialkylidene ketones, featuring skipped diene moieties, with high regioselectivities and stereoselectivities. The reaction is distinct from previously reported, rhodium-catalyzed aldehyde−allene 1:2 coupling to afford β,γ-dialkylidene ketones bearing 1,3-diene moieties. The present hydroacylative dimerization involves a unique allene/allene oxidative cyclization mode to form a C1−C2 linkage between the allene molecules.