Abstract: | The activation of C? H bonds has revolutionized modern synthetic chemistry. However, no general strategy for enantiospecific C? H activation has been developed to date. We herein report an enantiospecific C? H activation reaction followed by deuterium incorporation at stereogenic centers. Mechanistic studies suggest that the selectivity for the α‐position of the directing heteroatom results from a four‐membered dimetallacycle as the key intermediate. This work paves the way to novel molecular chemistry on nanoparticles. |