Hydrogel-based electronics are ideally suited for neural interfaces because they exhibit ultracompliant mechanical properties that match that of excitable tissue in the brain and peripheral nerve. Hydrogel-based multielectrode arrays (MEA) can conformably interface with tissues to minimize inflammation and improve the reliability to enhance signal transduction.However, MEA substrates composed of swollen hydrogels exhibit low toughness and low adhesion stability when laminated on the tissue surface and also present technical challenges for processes commonly employed in MEA fabrication. Here, we describe a new strategy to fabricate ultracompliant MEA based on aqueous-phase transfer printing. This technique employs redox active adhesive motifs in hygroscopic polymer precursors that simultaneously form hydrogels through sol-gel phase transitions and bond to underlying microelectronic structures. Specifically, in situ gelation of 4-arm-polyethylene glycol-grafted catechol [PEG-Dopa]4 hydrogels induced by oxidation using Fe 3+ produces conformal adhesive contact with the underlying MEA, robust adhesion to electronic structures, and rapid dissolution of watersoluble sacrificial release layers. MEA are then integrated on hydrogel-based substrates to produce free standing ultracompliant neural probes, which are then laminated to the surface of the dorsal root ganglia in feline subjects to record single-unit neural activity.