As one of the most important noble metals, Pd species including Pd 0 and PdO x based catalysts have exhibited excellent catalytic activity toward methane combustion at relatively low temperatures. [2,3] During manufacturing applications the active Pd species were usually loaded on metal oxides (MO x ) supports via the traditional deposition precipitation [4,5] or impregnation [6,7] methods in which good Pd dispersion could result in ideal initial catalytic activity. However, these strategies brought an obvious drawback that the as-obtained Pd nanocatalysts with overexposed active centers often exhibited unsatisfied thermal stability caused by sintering. To solve this problem, kinds of Pd@MO x core(yolk)@shell nanostructures [8][9][10] and Pd-metal alloys [11][12][13] have been successfully investigated to improve anti-sintering ability of Pd despite the catalytic active centers might be partially blocked, so it seems hard to reconcile activity and stability. Moreover, most of the Pd@MO x core@shell nanostructures and Pd-metal alloys are prepared by toxic and complex organic routes that limit mass production for application.From a widely accepted viewpoint of catalysts design, there should be enough exposed active centers and highly dispersed Pd species as catalytic sites, strong coupling between Pd and MO x to produce effective synergistic effects, [14,15] and welldefined MO x nanostructures as supports to get large specific surface areas and rational pore distributions. [16][17][18][19][20] Obviously, the properties of MO x supports greatly determined the final performance of Pd catalysts. [21,22] 2D nanosheets (NSs) have been considered as good supports to anchor Pd, which are of large aspect ratios and high specific surface areas. [23][24][25] Such 2D material supported hybrid nanocatalysts have been successfully used in photocatalysis [26] and electocatalysis, [27,28] showing potential applications for renewable energy production and environment remediation. [29,30] However here comes a new question that these reported ultrathin 2D NSs are mainly based on carbon materials, [31,32] metal chalcogenide, [33] and transition metal hydroxides [34,35] that are hard to survive from calcination caused by thermal decomposition and meanwhile transformed into oxides. As a result, the initial 2D nanostructures were thoroughly damaged into heavily aggregated nanoparticles (NPs), leading to bad catalytic performance during heterogeneous catalysts.For years we have been focusing on preparation of noble metal or MO x catalysts with well-defined nanostructures via nonorganic routes, especially for those CeO 2 encapsulated ones. [36][37][38][39][40] CeO 2 is of excellent oxygen storage/release capacity, Efficient utilization of methane via catalytic complete combustion is a very important pathway to realize energy efficiency and pollution reduction. From the viewpoint of structural design, herein a green water-phase route is developed to prepare ultrathin Co(OH) 2 nanosheet supported Pd catalysts. As a platform, the as-obtained...