The mechanical properties of nanometer-thick graphite film (NGF) and graphene were characterized using a bulge test. Young’s modulus, fracture stress, residual strain and stress of the NGF were measured. The NGF was synthesized on a Ni/SiO2/Si substrate using a chemical vapor deposition system. Large-area freestanding NGF was prepared via camphor transfer. Young’s modulus, fracture stress and fracture strain of the NGF were 106[Formula: see text]GPa, 462[Formula: see text]MPa, and 0.3%, respectively, confirming that the bulge test is a very useful technique for evaluating the mechanical properties of NGF. A bulge test was performed to evaluate the mechanical properties of graphene with a free-standing poly (bisphenol A carbonate) (PC)/graphene layer. Large-area freestanding PC/2D material layers were prepared by peeling-off and stamping. The PC layer was used as the supporting layer in this study. Young’s modulus of graphene was calculated from Young’s modulus of the PC/2D material layers and PC layers using the rule of mixtures. Young’s modulus of the graphene was 260[Formula: see text]GPa. The results of this study confirm the efficacy of the bulge test for determining the mechanical properties of nanometer-thick films and 2D materials, including graphene.