Pseudo-single atom Pt catalysts have achieved an excellent selectivity to branched paraffins and cycloalkanesi nn-hexaner eforming here. Highly dispersed platinum in single-atom and small clusters made up of severals eparated atoms wasp roduced under the inducemento fSno rZ ra sp romoting components. The Sn or Zr oxides were topologically transformed from layered double hydroxides as precursors, and thus homogeneouslyd ispersed owing to the confinemento ft he brucitelike lattices. The lattice confinementa lso caused the promoter sites charge-transferred, affording electron-rich (Sn) or electron-defected (Zr) sites on the surface, therebyf acilitating the inducement to Pt sites. This strategy provides an effective and feasible alternative for the facile preparation of highly dispersed metal catalysts. In n-hexane reforming, as electivity of up to 95 %t ob ranched paraffins and cycloalkanesw as obtained with the pseudo-single-atomPtcatalysts.The catalytic reforming of straight-chain paraffin to branched paraffin and/orc ycloalkanesi samajor petroleum refining process for the production of high-octaneg asoline. The hydrogenolysis byproducts, however,n eed to be avoided for the atomeconomy.[1] The aromatic compounds are also undesired, as environmental regulations limit the carcinogenic components in gasoline.[2] The reformingp rocess is industrially accomplished by use of supported platinum catalysts.[3] It is critical to enhance the dispersiono fP ta toms for sake of product selectivity.[1b, 4] Large Pt ensemblesh ave been found to be active for the hydrogenolysis to form C1-C5 [5] by the factor of a3Dstruc-ture, the so-called B5 sites.[5b] The 6-fold coordinated step-like sites favor the dehydrocyclization to produce aromatic compounds.[6] To improve Pt dispersion, many efforts have been made during the past decades. The support properties [7] prove important for the dispersiono fP ts ites, such as the surface properties, [7a] porouss tructures, [7b] or surfaced efectt ypes.[7c] Pt loading is also ac ritical factor, [8] including Pt precursor, [8a,b] loaded amount, [8b] and loading method. [8b,c] Strengthening the Pt-support interactions helps improving Pt dispersion as well. [9] The formation of an ew interaction (e.g. Pt-(ONa) x -SiO 2 )b ya ddition of sodium ion [9a] or an enhanced Pt-support interaction by addition of rare earth ions (e.g. Tm)[9b] has improved the dispersion of Pt to cluster size. Addition of Re, Sn, or Ge as promoter is especially efficacious because, in addition to altering the electron density of Pt, [10] the promoter component separates Pt atomsf rom large aggregates by forming Pt x Ma lloys [11] or Pt-promoter oxidesislands. [12] Recently,( pseudo)-single-atom noblem etal catalysts have attracted significant attention owing to their remarkable catalytic properties. [13][14][15][16][17][18] Ac atalystw ith Pt atoms completely exposed to MgO surface has been obtained through am ass-selected soft-landing technique, in which each Pt atom counts for CO oxidation.[13] Isolated A...