The high potential of metal-doped fullerenes (C 60 ) as hydrogen-storage materials has recently been discussed intensively. [1][2][3][4][5][6] Owing to its unique mechanical properties, such as high surface area and porosity, C 60 is believed to be one of the most promising hydrogen-storage systems. Utilization of noble or transition metals as dopants for C 60 will lead to stronger interactions with hydrogen molecules based on Dewar-Kubas interactions, reaching the target of the hydrogen-adsorption capacity set by the US Department of Energy (6.5 wt%). [4][5][6] However, so far all of the reports on noble or transition metal-doped C 60 are restricted to theoretical discussions because of the difficulties in the fabrication arising from the highly cohesive characteristics of metal atoms and, thus, the actual fabrication of these materials has been highly desired.Noble metal-doped C 60 will also provide a route to addressing the possibility of superconductivity in these systems, suggested by the observation of a gap opening at the Fermi level of a C 60 monolayer on Ag, [7] which triggered a large number of studies on the structural and electronic properties of noble metal-C 60 systems. [8][9][10] Since most studies have been restricted to the 2D configuration (bilayer) of noble metals and C 60 because of cohesive characteristics of noble metals, [8][9][10][11][12][13][14] it has been difficult to address directly the possibility of superconductivity in these systems. Furthermore, several puzzling issues, such as various bonding characteristics between metals and C 60 [13,14] or negative and positive changes in work functions depending on substrates, [14] have not yet been well understood, thus, the noble metal-doped C 60 is expected to serve as a 3D platform for further investigation of these issues.Despite these promising and intriguing properties, fabrication of noble or transition metal-doped C 60 has been one of the fundamental challenges. The high cohesive energy of metals (e.g., 3.48, 2.93, and 3.81 eV, for Cu, Ag, and Au, respectively) [15] compared to that of alkali or alkaline earth metals (e.g., 1.11, 0.93, 1.87, and 1.90 eV, for Na, K, Sr, and Ba, respectively) [15] leads to aggregation of metal atoms separated from a C 60 phase. The co-deposition of metals and C 60 is reported as an effective way to fabricate metal-C 60 mixed films. [16,17] In these previous studies, however, metals and C 60 were deposited on a substrate kept at room temperature, where both metal atoms and C 60 molecules have quite high mobility, resulting in aggregation of metals separated from a C 60 phase.To suppress the diffusion and aggregation, we utilize a substrate maintained at low temperature in the present study. We focus on the Ag-C 60 system because not only the possibility of novel superconductivity [7] but also the improvement of hydrogen adsorption with Ag has been reported. [18,19] In addition, the ion radius of Ag þ (0.129 nm) is comparable with that of alkali or alkaline earth metals, ranging from 0.090 to 0.181 nm, w...