In this work we report on the photocurrent increasing obtained by using thylakoid membranes “wired” with an osmium redox polymer (OsRP) immobilized onto screen-printed carbon and gold electrodes (SPCEs and SPAuEs), modified with gold microparticles (AuMPs) and gold nanoparticles (AuNPs). Both AuMPs and AuNPs were electrodeposited by using the same electrodeposition method, in order to study the influence of different electrode surface morphologies, namely AuMPs and AuNPs, on the photocurrent generated when illuminated with light with an intensity equivalent to that of sunlight (400 W m−2). AuMPs/SPCEs showed the highest current density (62.5 μA cm−2) upon illumination probably due to a higher capacitive current directly related to the enhanced electroactive area (AEA) and roughness factor (ρ). Finally, the so modified electrodes AuMPs/SPCE and AuNPs/SPAuE were characterized by using scanning electron microscopy (SEM) showing a different surface morphology, resulting in a higher surface roughness for AuMPs/SPCE compare to AuNPs/SPAuE therefore an intimate interaction between the large thylakoid membrane and the AuNPs. A high photocurrent density of 62.5 μA cm−2 was generated at a light intensity of 400 W m−2.