A unique microfluidics approach for functional hydrogel patterning with multilayered heterogeneous structures is presented. Prepolymer solution droplets with differentiated sodium acrylate concentrations are dispensed/printed in a wetting‐controlled “two‐parallel plate” (TPP, like a Hele‐Shaw Cell) system. The gelation within the system enables hydrogel bilayer structures with reconfigurable 3D deformations driven by in‐plane and through‐thickness heterogeneity under stimuli‐responsive mask‐less swelling/deswelling. The cooperation between swelling mismatch of functional groups results in a higher complexity of 3D reconfiguration in responding to discrete levels of stimulation inputs. This facile patterning technology with an in‐built ionic hierarchy can be scaled up/down with advanced transducing functionalities in various fields
