Graphene has tremendous potential in future electronics due to its superior force, electrical, and thermal properties. However, the development of graphene devices is limited by its complex, high‐cost, and low‐efficiency preparation process. This study proposes a novel laser bidirectional graphene printing (LBGP) process for the large‐scale preparation of patterned graphene films. In LBGP, a sandwich sample composed of a thermoplastic elastomer (TPE) substrate, carbon precursor powder, and a glass cover is irradiated by a nanosecond pulsed laser. The laser photothermal effect converts the carbon precursor into graphene, with partial graphene sheets deposited directly on the TPE substrate and the remaining transferred to the glass cover via a laser‐induced plasma plume. This method simultaneously prepares two face‐to‐face graphene films in a single laser irradiation, integrating synthesis, transfer, and patterning. The resulting graphene patterns demonstrate good performance in flexible pressure sensing and Joule heating, showcasing high sensitivity (7.7 kPa−1), fast response (37 ms), and good cycling stability (2000 cycles) for sensors, and high heating rate (1 °C s−1) and long‐term stability (3000 s) for heaters. It is believed that the simple, low‐cost, and efficient LBGP process can promote the development of graphene electronics and laser manufacturing processes.