The light-dependent reactions of photosynthesis use light energy to generate photoelectrons traveling through the thylakoid membranes (TMs). Extracting the photoelectrons from the TMs to form bioanodes can have various applications. Most studies focus on modifying the electrode materials to increase the collected photocurrent. Seldom studies have investigated how the orientation of the TMs influences photocurrent collection. In addition, the formation of reactive oxygen species (ROS) during photosynthesis is a challenge for stable photocurrent generation. Here, we enhanced the photoelectron transfer from the TMs to electrodes by depositing expanded thylakoids as planar supported membranes onto an electrode. The high contact area between the external electrodes and TMs per unit mass of thylakoid allows the thylakoid to more effectively transfer electrons to the electrodes, thereby reducing the free electrons available for the ROS generation. We expanded the naturally stacked thylakoids into liposomes through osmotic pressure and dropcasted them onto an Au electrode. The electrochemical impedance measurement showed that the supported membrane bioanode formed by the expanded liposomes had a lower photoelectron transfer resistance. Additionally, we observed that the expanded TM bioanode provided a higher photocurrent and was more durable to air/water interfacial tension. These results suggest that the effective contact between the expanded TM and electrodes can lead to more efficient electron transfer and increase the system robustness. The photo fuel cell (PFC) made by the expanded TM bioanode had a higher open-circuit voltage than the one made by the stacked TM bioanode. Interestingly, we found that PFCs made of high-load TM bioanodes had fast photocurrent decay under continuous operation at high cell voltages. The poor contact of large numbers of TMs with the electrodes at the high-load TM bioanodes could cause more ROS accumulation and therefore decreased the operational stability, supporting the importance of effective contact between TMs and the electrodes.