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              <p>The key importance of the 3D structure of therapeutic and bioactive compounds has been highlighted by recent research. Despite their potential in pharmaceutical development, creating such complex structures, particularly those incorporating tetrasubstituted stereocenters, remains a formidable challenge. Recently, α-cyanocarbanionic metal complexes have emerged as promising nucleophilic intermediates, due to the broad functionalization potential of the nitrile group. Herein, we present an optimized Pd/Cu dual catalytic system that enables the allylic alkylation of secondary and tertiary nitriles under mild conditions, using chiral metal complexes. This strategy offers good to high levels of enantioselectivity (ee up to 91%). Mechanistic investigations, supported by DFT calculations, underscore the essential role of dual catalysis, wherein the orthogonal activation of Pd and Cu partners synergistically governs both reactivity and enantioselectivity. To demonstrate the synthetic utility of this newly developed methodology, the transformation of nitrile-containing compounds was also explored.</p>
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