Intentional generation, amplification, and discharging of chemical gradients is central to many nano- and micromanipulative technologies. We describe a straightforward strategy to direct chemical gradients inside a solution via local photoelectric surface charging of organic semiconducting thin films. We observed that the irradiation of carbon nitride thin films with ultraviolet light generates local and sustained surface charges in illuminated regions, inducing chemical gradients in adjacent solutions via charge-selective immobilization of surfactants onto the substrate. We studied these gradients using droplet force gradient sensors, complex emulsions with simultaneous and independent responsive modalities to transduce information on transient gradients in temperature, chemistry, and concentration via tilting, morphological reconfiguration, and chemotaxis. Fine control over the interaction between local, photoelectrically patterned, semiconducting carbon nitride thin films and their environment yields a new method to design chemomechanically responsive materials, potentially applicable to micromanipulative technologies including microfluidics, lab-on-a-chip devices, soft robotics, biochemical assays, and the sorting of colloids and cells.