In this work, we successfully prepare two-dimensional ultrathin single-crystalline platinum nanodendrites (PtNDs) with precisely controlled generation (size) through a surfactant-directed solution-phase synthesis. The amphiphilic surfactant of C₂₂H₄₅–N⁺(CH₃)₂CH₂COOH (Br^–) acts as the structure-directing template and facet-capping agent simultaneously to kinetically engineer in-the-plane epitaxial growth of Pt nanocrystals along selectively exposed {111} facets into ultrathin PtNDs. A novel formation mechanism defined as crystalline facet-directed step-by-step in-the-plane epitaxial growth, similar to the synthesis of organic dendrimers, is proposed on the basis of the nanostructure and crystalline evolution of PtNDs. The generation growth process is readily extended to precisely engineer the generation of PtNDs (from 0 to 25) and can also be utilized to grow other noble metal NDs (e.g., PdNDs and AuNDs) and core–shell Pt–Pd NDs. Because of the structural advantages, ultrathin PtNDs exhibit enhanced electrocatalytic performance toward hydrogen evolution reaction.