Overlayer Pt on Ni (Ni@Pt) or Co (Co@Pt) were synthesized and tested for H-2 generation from APR of lactose. H-2 chemisorption descriptor showed that Ni@Pt and Co@Pt overlayer catalysts had reduced H-2 adsorption strength compared to a Pt only catalyst, which agree with computational predictions. The overlayer catalysts also demonstrated lower activity for ethylene hydrogenation than the Pt only catalyst, which likely resulted from decreased H-2 binding strength decreasing the surface coverage of H-2. XAS results showed that overlayer catalysts exhibited higher white line intensity than the Pt catalyst, which indicates a negative d-band shift for the Pt overlayer, further providing evidence for overlayer formation. Lactose APR studies showed that lactose can be used as feedstock to produce H-2 and CO under desirable reaction conditions. The Pt active sites of Ni@Pt and Co@Pt over layer catalysts showed significantly enhanced H-2 production selectivity and activity when compared with that of a Pt only catalyst. The single deposition overlayer with the largest d-band shift showed the highest H-2 activity. The results suggest that overlayer formation using directed deposition technique could modify the behavior of the surface metal and ultimately modify the APR activity.