Summary The crystal structure of 2, 6-bis (lithiumtrimethylsilylmethyl) pyridine· 2TMEDA, which is readily obtained by metallation of 2, 6-(Me 3 SiCH 2) 2 C 5 H 3 N, exhibiting double (η 3-aza-allyl)-lithium bonding, represents a beautiful example of C− Li+ N− Li+ C− charge communication, and confirms the predictions of theory.