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Reported in this work is a synergistic ternary achiral picolinaldehyde‐Zn(II)‐chiral palladium complex system for the highly enantioselective α‐allylation of N‐unprotected amino esters. By utilizing a variety of allylic carbonates or vinyl benzoxazinanones as substrates, α‐allyl α‐amino esters were obtained in high yields (up to 96 %) with high enantioselectivities (up to 98 % ee). Control experiments...