An enantio- and diastereodivergent [2+2+1] annulation reaction of allyl ketones, acidic methylene compounds, nitroalkenes to assemble highly functionalized cyclopentanes from readily available substances enabled by asymmetric relay catalysis chiral bifunctional squaramide palladium complex has been established. This method showcases that ketones can serve as latent 1,2-dication synthons via a l...