Designing and tailoring metal-support interaction in Ni-based catalysts with plentiful interfacial sites is of significant interest for achieving a targeted catalytic performance in dry reforming of methane (DRM), but remains as a challenging task. In this work, Ni/Al₂O₃ and Ni/CeO₂-Al₂O₃ catalysts with the same strong metal-support interaction (SMSI) but distinct interface structure are developed by an improved evaporation-induced self-assembly method using pseudobohemite gel as aluminum source. Ni/CeO₂-Al₂O₃ exhibits superior catalytic activity and stability in DRM in comparison with Ni/Al₂O₃. The highest CH₄ and CO₂ conversion reaches at 71.4% and 82.1% for Ni/CeO₂-Al₂O₃, which are higher than that of 64.3% and 75.6% for Ni/Al₂O₃ at 700 °C. The SMSI effect in Ni/CeO₂-Al₂O₃ provides more active interfacial sites with less coke deposition, and promotes the generation of active formate species which are the key intermediates for DRM. The findings of the present work could possibly pave the way for fabricating catalysts with SMSI strategy for efficient heterogeneous catalysis.