A new and unique alloy formulation design strategy has been developed in order to fabricate thin-layered metallic glasses (TLMGs) with superior fracture resistance and low coefficient of friction (COF) during the nanoscratching test. Due to the outstanding properties, TFMG could be applied for different uses, such as for surface coating, biomedical, bioimprinting, electronic devices, spacecraft, and railway, all of which need surface fracture resistance. The fabricated Zr-based metallic glass was prepared from Zr, Al, Cu, Ni, and Ag above 99.9 Wt % in purity by arch melting techniques. TFMGs were coated on silicon wafer by sputtering the vapor deposition method from bulk metallic glass then annealed below glass transition temperature T g ∼ 450 °C for 10, 30, and 60 min. Nanoindentation and nanoscratch tests were used to investigate nanomechanical and nanotribological properties, and atomic force microscopy (AFM) was used to examine the surface morphology and microstructures of TLMG. The nanoindentation data indicated that the average hardness of metallic glasses increased from 9.75 (as-cast MG) to 13.4 GPa (annealed for 60 min). Coefficients of friction for the cast sample, annealed for unannealed, 10, 30, and 60 min, were 0.062, 0.049, 0.039, and 0.03, respectively, as well as the wear depths were 201. 56, 148.43, 37.32, and 25.27 nm, respectively. These studies show that the coefficient of friction and wear rate decreases when the annealing time increases as a result of atomic reordering and structural relaxation that occurred at longer annealing times. Furthermore, continuous wear process, wear depth, wear track volume, and contact area decrease with increasing annealing time. This study can be used to design protocols to prepare novel TLMGs, which have outstanding mechanical and tribological properties for engineering materials applications.