In general, for racemic reactions, the best yields of product were obtained using achiral urea or squaramide catalysts (Scheme 2). For scalemic reactions, the best enantioselectivities were obtained using chiral thiourea catalysts C, D, or E (Table and Scheme 2), but the choice of catalyst was substrate-dependent and empirically determined. A variety of functional groups were well-tolerated, including aromatic ethers, halogens, and CF3 moieties (Scheme 2, Products 3-15). With substrates bearing large substituents ortho to the nitro-olefin, excellent yields could be obtained using our racemic protocols, but the yields and enantioselectivities suffered in the scalemic reactions (Scheme 2, Products 16-18). We will revisit this issue during our discussion of enantioinduction (vide infra). Certain substrates failed to give product in reasonable yields, including nitrolefins 19-20, α,β-unsaturated ester 21, and α,β-unsaturated ketone 22.