The long-term vision for the research directions of the nbml-E3 group is to design, develop and deploy a bio-hybrid PEC cell via systematic integration of complex IM/MO NCs and NAs, as energetically tuned photocatalysts (WOC) and electrocatalysts (HER), with PS I as the biological electron mediator for efficient solar water splitting. The design of a single junction semiconductor based photocatalyst with ideally tuned band gaps (visible light absorption), band edge potentials, and interfacial electron transfer kinetics that can promote efficient and stable solar water splitting process is formidable. In contrast, the ultra-fast photoactivated electron-hole separation within PS I along with its 680 nm excitation wavelength can effectively increase the absorption band while improving the charge transport properties through reduced recombination losses. Hence, we seek to interface our research on facile and cost-effective synthesis of advanced nanocatalysts via tandem LASiS-GRR with our current expertise in the solar photochemistry of energy harvesting PS I to make PS I-inorganic photocatalyst interfaces as photoanode materials that can mimic nature’s route for producing solar fuels that has been one of the primary sources of energy on earth since the evolution of oxygenic photosynthesis over 2 billion years ago. Such bio-inspired photonic devices, when wired up with well-designed electrocatalysts and photocatalysts, provide the future promising potentials for the “holy grail” of solar water splitting via “artificial photosynthesis.”