We successfully prepared a highly porous graphene on carbon cloth (PG/CC) via an electrophoretic deposition process. With this process, in order to obtain high porous graphene on carbon cloth, fine-size graphene should be used. When large-size graphene was used, carbon cloth was only covered by graphene (G/CC) without porous surface. PG/CC was used as electrodes for Flexible All-Solid-State Supercapacitors (FASSSs). The porous structure of PG/CC electrode significantly increased the surface area of graphene and thus the specific capacitance (79.19Fg−1 for PG/CC and 32.35Fg−1 for G/CC). The macroscopic porous morphology of carbon cloth as the electrode matrix enhanced the integration between electrode and electrolyte, which is favorable for the ion diffusion and electron transport. The excellent mechanical stability and flexibility of PG/CC ensures the device with good flexibility. The resultant PG/CC based FASSSs showed high specific capacitance, good cycling stability, and enhanced energy density and power density.