(R)- and (S)-CpMo(NO)(eta3-methallyl)((S)-(+)-10-camphorsulfonate) (Cp = cyclopentadienyl) have been prepared and separated. This provides a route for resolution of the chiral molybdenum center and allows the isolation of enantiomerically pure CpMo(NO)(eta3-methallyl)X (X = Cl, Br,I)complexes. Reaction of (+)-CpMo(NO)(eta3-methallyl)Cl with benzaldehyde in the presence of methanol yields (S)-(-)-3-methyl-1-phenyl-3-buten-1-ol, in >98% ee. (+)-CpMo(NO)(eta3-methallyl)I (1) was found to have the R configuration by X-ray crystallography.