Furfural was effectively synthesized from xylose in a one pot manner by the combined use of Ni2+-modified gamma-Al2O3 (Al2O3-Ni-Al layered double hydroxide (LDH)) and a sulfonated resin (Amberlyst-15) at 373 K (46% yield). The addition of Ni2+ onto gamma-Al2O3 generated the bi-functional sites for Lewis acid gamma-Al2O3 and Bronsted base Ni-Al LDH at close boundary, and these facilitate the xylose isomerization into xylulose and/or ribulose to afford good yield of furfural after successive dehydration of generated ketopentoses on Amberlyst-15.