In this research, we constructed a controlled chamber pressure CVD (CP-CVD) system to manipulate graphene's domain sizes and shapes. Using this system, we synthesized large (~4.5 mm(2)) single-crystal hexagonal monolayer graphene domains on commercial polycrystalline Cu foils (99.8% purity), indicating its potential feasibility on a large scale at low cost. The as-synthesized graphene had a mobility of positive charge carriers of ~11,000 cm(2) V(-1) s(-1) on a SiO(2)/Si substrate at room temperature, suggesting its comparable quality to that of exfoliated graphene. The growth mechanism of Cu-based graphene was explored by studying the influence of varied growth parameters on graphene domain sizes. Cu pretreatments, electrochemical polishing, and high-pressure annealing are shown to be critical for suppressing graphene nucleation site density. A pressure of 108 Torr was the optimal chamber pressure for the synthesis of large single-crystal monolayer graphene. The synthesis of one graphene seed was achieved on centimeter-sized Cu foils by optimizing the flow rate ratio of H(2)/CH(4). This work should provide clear guidelines for the large-scale synthesis of wafer-scale single-crystal graphene, which is essential for the optimized graphene device fabrication.