In this study, we report an instantaneous polymeric adhesive with high strain tolerance (termed as iPASTE) even in a stretchable human–machine interface. The iPASTE consists of two biocompatible and eco-friendly polymers, linearly oligomerized green tea extracts, and poly(ethylene glycol) for densely assembled networks via dynamic and reversible hydrogen bonds. Based on the strain-tolerant adhesion of iPASTE, a subaqueous interactive human–machine interface integrated with a robot arm and a gold nanomembrane strain-sensitive electronic skin can precisely capture a slithery artificial fish by using finger gesture recognition.