Treatment of 2-bromo-4,6-dimethylphenylisocyanide (1a) with 1.2 equiv of n-BuLi in THF at -78 degrees C provided an o-isocyanoaryllithium intermediate, which reacted with aldehydes, nitroalkenes, and trimethylchlorosilane to give the corresponding products in good yields. Asymmetric conjugate addition to nitroalkenes in the presence of (1)-sparteine in toluene gave the products with good stereoselectivities up to 85% ee.