Neural
interfaces are the fundamental tools to understand the brain
and cure many nervous-system diseases. For proper interfacing, seamless
integration, efficient and safe digital-to-biological signal transduction,
and long operational lifetime are required. Here, we devised a wireless
optoelectronic pseudocapacitor converting the optical energy to safe
capacitive currents by dissociating the photogenerated excitons in
the photovoltaic unit and effectively routing the holes to the supercapacitor
electrode and the pseudocapacitive electrode–electrolyte interfacial
layer of PEDOT:PSS for reversible faradic reactions. The biointerface
showed high peak capacitive currents of ∼3 mA·cm
–2
with total charge injection of ∼1 μC·cm
–2
at responsivity of 30 mA·W
–1
, generating
high photovoltages over 400 mV for the main eye photoreception colors
of blue, green, and red. Moreover, modification of PEDOT:PSS controls
the charging/discharging phases leading to rapid capacitive photoresponse
of 50 μs and effective membrane depolarization at the single-cell
level. The neural interface has a device lifetime of over 1.5 years
in the aqueous environment and showed stability without significant
performance decrease after sterilization steps. Our results demonstrate
that adopting the pseudocapacitance phenomenon on organic photovoltaics
paves an ultraefficient, safe, and robust way toward communicating
with biological systems.