possess high electric conductivity, improved chemical & physical stability, and ultrahigh mass transfer efficiency. Therefore, in the past several decades, 1D carbon nanostructures have been exploited as robust materials in catalysis, [2] either as active materials or functional matrices to anchor various metal species. [3] To improve the application potential, introduction of heteroatoms into the 1D carbon nanostructure is essential as it allows to effectively engineer the electronic structure. [4] P and N are the popular choices but incorporating these heteroatoms into 1D carbon nanostructures normally needs multiple synthetic steps. It is important to develop simple and controllable method to synthesize heteroatom-doped 1D carbon nanostructures with superior abilities in cutting-edge applications.Alkene hydrosilylation is the addition of SiH to the unsaturated bonds, which is one of the most important chemical reactions to produce the organosilicon compounds. Platinum (Pt) homogeneous catalysts, namely the Speier Pt catalyst and Karstedt Pt catalyst, [5] have been the most popular choice in alkene hydrosilylation [6] and consume nearly 5.6 tons of platinum annually in silicone industry. [7] Unfortunately, the side reactions, including the alkene isomerization and dehydrogenative silylation, normally accompany with the main reaction, and expensive purification is needed. [8] Moreover, the additional side reactions occur due to the formation of colloidal Pt species, [9] and the recycling of Pt homogeneous catalyst is a wellknown challenge. This not only increases the production cost but also introduces impurities to the final product. [10] In this context, single-atom catalysts, which contains atomic dispersion of active metallic species on a support, have been recently developed to overcome these challenges. It exhibits an unexpected catalytic performance, while it also owns great convenience in recovery. The synthesis of the atom support is the key step to obtain this interesting material.More recently, based on P 2 O 5 chemistry, we successfully synthesized metal-free COP functionalized carbon-nanofiber assemblies. [11] This unique carbon nanostructure was proven to possess exceptional adsorption properties, a useful pre-requirement for catalysis. The outcome further inspired us to upgrade this in situ P 2 O 5 chemistry to introduce novel functional groups to 1D carbon nanostructure. Unfortunately, the previously Single-atom catalysts have become a popular choice in various catalysis applications, as they take advantages of both homogeneous catalysis (e.g., high efficiency) and heterogeneous catalysis (e.g., easy catalyst recovery). The atom support plays an indispensable role in anchoring atomic species and interplaying with them for ultimate catalytic performance. Therefore, development of new support materials for superior catalysis is of great importance. Here the synthesis of carbon nanofibers based on the reaction between phosphorus pentoxide (P 2 O 5 ) and N-methyl-2-pyrrolidone (NMP) is reporte...