(Graph　Presented)　Cu/ZnO/Al2O3　catalysts　with　different　compositions　were　prepared　from　Cu-Zn-Al　layered　double　hydroxides　(LDHs)　and　tested　for　the　water-gas　shift　reaction.　LDHs　were　synthesized　by　the　coprecipitation　method,　and　Cu-Zn-Al　LDHs　or　Cu-Al　LDHs　could　be　formed　depending　on　the　(Cu　+　Zn)/Al　atomic　ratio.　Upon　calcination,　LDHs　decomposed　to　form　mixed　metal　oxides　consisting　of　CuO,　ZnO,　ZnAl2O4,　CuAl2O4,　and/or　amorphous　Al2O3.　After　reduction,　well　dispersed　Cu　metal　particles　with　18-48%　dispersion　and　2-6　nm　size　were　formed.　It　was　observed　that　the　initial　activity　of　Cu/ZnO/Al2O3　catalysts　was　proportional　to　the　number　of　surface　Cu0　atoms　and　the　30%Cu/Zn1Al　catalyst　showed　the　highest　activity.　Moreover,　this　optimum　catalyst　exhibited　better　activity,　thermal　stability,　and　long-term　stability　than　a　commercial　Cu/ZnO/Al2O3　catalyst.　It　was　considered　that　a　synergetic　effect　between　Cu　metal　and　ZnAl2O4　spinel　might　exist　and　play　a　key　role　for　the　high　catalytic　performance.　©　2017　American　Chemical　Society.