Developing effective nickel-based catalysts in hydrogenation of pyrolysis gasoline (PyGas) is of great importance in chemical industry. Herein, we report a facile fabrication of Al2O3-supported NiRu bimetallic catalysts, with Ru content ranging from 0.01 wt% to 0.1 wt%, by reducing of precursors of Ni2+Ru3+Al3+ -containing layered double hydroxides (NiRuAl-LDHs) in flowing hydrogen. Their catalytic performance was evaluated by styrene hydrogenation, a model reaction in industrial hydrogenation of PyGas (abbreviated as PyGasMF). The LDH precursors initially in situ grow on the surface of microspherical gamma-Al2O3 supports. Doping Ru3+ in LDH main layers promotes reduction of Ni2+ by hydrogen spillover and decreases significantly the size of Ni metal particles, and NiRu alloy particles are formed during the reduction. Substitution of an appropriate amount of Ni for Ru enhances the catalytic activity and stability in styrene hydrogenation, demonstrating a synergistic effect of Ni and Ru on hydrogenation reactivity.