<abstract abstract-type="main" xml:lang="en"> <title>Abstract</title> <p>A chiral N‐heterocyclic carbene‐catalyzed a<sup>3</sup> → d<sup>3</sup>‐umpolung addition of α, β‐enals to racemic α‐keto esters gives access to γ‐butyrolactones with high regio‐, diastereo‐, and enantiocontrol.</p> </abstract>