Optically driven extracellular electronic neuromodulation devices are a novel tool in basic research and offer new prospects in medical therapeutic applications. Optimal operation of such devices requires efficient light capture and charge generation, effective electrical communication across the device’s bioelectronic interface, conformal adhesion to the target tissue, and mechanical stability of the device during the lifetime of the implant - all of which can be tuned by spatial structuring of the device. We demonstrate a 3D structured opto-bioelectronic device – an organic electrolytic photocapacitor spatially structured by depositing the active device layers on an inverted micropyramid-structured substrate. Ultrathin, transparent, and flexible micropyramid-structured foil was fabricated by chemical vapour deposition of parylene C on silicon moulds containing arrays of inverted micro pyramids, followed by a peel-off procedure. The capacitive current delivered by the devices showed a strong dependency on the device structuring. The device performance was evaluated by numerical modelling, enabling functional optimization of the devices for specific purposes. Additionally, micropyramid structuring is expected to affect the device-tissue adhesion and afford a level of stretchability to otherwise flexible but non-stretchable parylene C foil substrates.