Autothermal dry reforming of methane (ATR-DRM) has gained considerable research attention for its application in the conversion of methane and carbon dioxide to valuable synthesis gas (syngas). However, granular Ni-based catalysts offer limited stability and durability when used in the dry reforming of methane (DRM). Here, the performance of a honeycomb-type Ni/Al2O3 structured catalyst during syngas production was investigated under ATR-DRM conditions. The catalyst was successfully prepared on an aluminum-fin substrate by a combination of sol-gel and electroless plating methods. The addition of oxygen during the DRM significantly enhanced the reforming performance and considerably suppressed coke deposition. Furthermore, the Ni/Al2O3 structured catalyst could reduce hot spot formation and improve energy efficiency. Therefore, ATR-DRM using a structured catalyst is a promising technology that promotes process intensification.