Switchable interfaces can deliver functionally reversible reactivity with their corresponding analytes, which allows one to positively respond to the activity of biological elements, including enzymes and other biomolecules, through an encoded stimulus. We have realized this by the design of stimuli-responsive graphene interfaces for the pH-encoded operation of bioelectronics. Herein, we have demonstrated stimuli-responsive graphene interfaces for the pH-encoded operation of bioelectronics. The resulting switchable interfaces are capable of the highly specific, on-demand operation of biosensors, which has significant potential in a wide range of analytical applications.