Two-dimensional (2D) nanomaterials have attracted much interest as promising candidates for next generation energy storage, electronics and catalytic applications, due to their unique topology and electronic structure. However, the development of an operable and versatile solution processing technique for simple fabrication of high-quality 2D nanosheets continues to present a significant challenge. Here, an ultrathin indium sulfide nanosheet is synthesized via a simple solution-phase reaction involving two steps: i) thermal decomposition of precursors to form a crystal nucleus; ii) growth of 2D nanosheets in a mixture of amino ligand and alkane solvent. The alkane, matching the amino ligand structure in terms of geometry, could assemble with the ligand to form a soft template and thus induce a 2D arrangement of the nucleus. Moreover, the chemical inertness of the alkane facilitated rotation of crystal seeds, resulting in anisotropic growth of the nanosheet. We further demonstrated that the geometrically matched alkane-assisted solution processing reaction could be applied to synthesize various 2D metal chalcogenides. Functionally, the acquired indium sulfide nanosheets, which possess high photoelectric activity, were introduced for fabrication of photoelectrodes capable of efficient photoelectrochemical water splitting. Our work opens up a new perspective toward the construction and potential applications for various 2D nanomaterials.

二维（2D）纳米材料因其独特的拓扑结构和电子结构而成为下一代储能，电子和催化应用的有前途的候选者，引起了人们的极大兴趣。然而，用于简单制造高质量2D纳米片的可操作且通用的溶液处理技术的发展继续提出了重大挑战。在此，通过涉及两个步骤的简单的溶液相反应，合成了超薄铟锡纳米片：i）前体的热分解以形成晶核；ii）在氨基配体和烷烃溶剂的混合物中生长2D纳米片。在几何学上与氨基配体结构匹配的烷烃可与配体组装形成软模板，从而诱导细胞核的二维排列。此外，烷烃的化学惰性促进了晶种的旋转，导致纳米片材各向异性生长。我们进一步证明，几何匹配的烷烃辅助溶液处理反应可用于合成各种2D金属硫属元素化物。在功能上，将获得的具有高光电活性的硫化铟纳米片引入到能够有效进行光电化学水分解的光电极的制造中。我们的工作为各种2D纳米材料的构造和潜在应用开辟了新的视角。我们进一步证明，几何匹配的烷烃辅助溶液处理反应可用于合成各种2D金属硫属元素化物。在功能上，将获得的具有高光电活性的硫化铟纳米片引入到能够有效进行光电化学水分解的光电极的制造中。我们的工作为各种2D纳米材料的构造和潜在应用开辟了新的视角。我们进一步证明，几何匹配的烷烃辅助溶液处理反应可用于合成各种2D金属硫属元素化物。在功能上，将获得的具有高光电活性的硫化铟纳米片引入到能够有效进行光电化学水分解的光电极的制造中。我们的工作为各种2D纳米材料的构造和潜在应用开辟了新的视角。