Integrating photosynthetic cell components with nanostructured materials can facilitate the conversion of solar energy into electric power for creating sustainable carbon-neutral energy sources. With the aim at exploring efficient photoinduced biocatalytic energy conversion systems, we have used an amidated carbon nanotube (aCNT) networked matrix to integrate thylakoid membranes (TMs) for construction of a direct electron transfer-driven biosolar cell. We have evaluated the resulting photobioelectrochemical cells systematically. Compared to the carboxylated CNT (cCNT)-TMs system, the aCNT-TMs system enabled a 1.5-fold enhancement in photocurrent density. This system offers more advantages including a reduced charge-transfer resistance, a lower open-circuit potential, and an improved cell stability. More remarkably, the average power density of the optimized cells was 250 times higher than that of reported analogue systems. Our results suggest the significance of physical and electronic interactions between the photosynthetic components and the support nanomaterials and may offer new clues for designing improved biosolar cells.