Owing to the maximum atom utilization efficiency, superior catalytic activity, and outstanding selectivity for many important reactions, single-atom catalysts (SACs) have shown great promise in heterogeneous and homogeneous catalysis. [1][2][3][4][5][6][7] Recently, various bottom-up strategies have been proposed to construct SACs. However, these methods usually suffer from tedious multistep processes, a massive waste of metal species, as well as disappointing yields, eventually hindering the development of SACs. [8][9][10][11] Even worse, elevated temperature treatment was an inevitable procedure in the bottom-up synthesis to reduce metal ions before forming well-defined single metal sites coordinated by defects, leading to high energy consumption and production cost. [12][13][14][15] The top-down strategies adopted for the synthesis of SACs, during which the cheap and available metal NPs or bulk metal Single-atom catalysts (SACs) feature the maximum atom economy and superior performance for various catalysis fields, attracting tremendous attention in materials science. However, conventional synthesis of SACs involves high energy consumption at high temperature, complicated procedures, a massive waste of metal species, and poor yields, greatly impeding their development. Herein, a facile dangling bond trapping strategy to construct SACs under ambient conditions from easily accessible bulk metals (such as Fe, Co, Ni, and Cu) is presented. When mixing graphene oxide (GO) slurry with metal foam and drying in ambient conditions, the M 0 would transfer electrons to the dangling oxygen groups on GO, obtaining M δ+ (0 < δ < 3) species. Meanwhile, M δ+ coordinates with the surface oxygen dangling bonds of GO to form MO bonds. Subsequently, the metal atoms are pulled out of the metal foam by the MO bonds under the assistance of sonication to give M SAs/GO materials. This synthesis at room temperature from bulk metals provides a versatile platform for facile and low-cost fabrication of