The need for 2D vertical graphene nanosheets (VGNs) is driven by its great potential in diverse energy, electronics, and sensor applications, wherein many cases a low-temperature synthesis is preferred due to requirements of the manufacturing process. Unfortunately, most of today's known methods, including plasma, require either relatively high temperatures or high plasma powers. Herein, we report on a controllable synthesis of VGNs at a pushed down low-temperature boundary for synthesis, the low temperatures (450 °C) and low plasma powers (30 W) using capacitively coupled plasma (CCP) driven by radio-frequency power at 13.56 MHz. The strategies implemented also include unrevealing the role of Nickel (Ni) catalyst thin film on the substrates (Si/Al). It was found that the Ni catalyst on Si/Al initiates the nucleation/growth of VGNs at 450 °C in comparison to the substrates without Ni catalyst. With increasing temperature, the graphene nanosheets become bigger in size, well-structured and well separated. The role of Ni catalysts is hence to boost the growth rate, density, and quality of the growing VGNs. Furthermore, this CCP method can be used to synthesize VGNs at the lowest temperatures possible so far on a variety of substrates and provide new opportunities in the practical application of VGNs.