The feasibility of continuous gas phase coupling of benzyl alcohol dehydrogenation with nitrobenzene hydrogenation for imine (N-benzylideneaniline) synthesis over mixtures of Cu/SiO2 and (TiO2, MgO) supported Au catalysts has been established. The catalysts were characterised in terms of specific surface area, pore volume, TPR, H2 chemisorption, STEM, XPS and TGA-DSC analysis. Au/TiO2 prepared by deposition-precipitation exhibited a narrower particle size distribution (1–6 nm) and smaller mean (3.2 nm) than Au/MgO (1–15 nm, mean = 7.7 nm) prepared by impregnation. Dehydrogenation of benzyl alcohol (to benzaldehyde) over Cu/SiO2 delivered a (ten-fold) higher rate than supported Au and Au/TiO2 exhibited a higher H2 chemisorption capacity and greater (by a factor of ten) nitrobenzene hydrogenation rate than Cu/SiO2 and Au/MgO. Inefficient hydrogen utilisation is demonstrated for the cross-coupling reaction over Cu/SiO2 alone and a temporal activity loss is linked to carbonaceous (benzoate) deposition (on the basis of XPS and TGA-DSC analysis). Incorporation of Au/TiO2 (and Au/MgO) with Cu/SiO2 increased the imine formation rate and H2 utilisation efficiency. The combination of Au/TiO2 with Cu/SiO2 served to circumvent Cu/SiO2 deactivation, resulting in enhanced stability with a four-fold increase in imine production and full H2 utilisation at Cu/Au = 10.