physical/chemical functionalization is capable of optimization of mechanical properties, [7] interfacial adhesion, [8] and self-healing ability of hydrogels. [9] These protocols normally introduced functional elements or structures that elicited physical/chemical interactions for the performance improvements of hydrogels. For example, polymeric nanoparticles from crystallization-driven self-assembly enabled mechanical improvements on hydrogel by physical hybridization with matrix. [10] Grafting silica nanoparticles to a double-network polymer also improved the hydrogel mechanical performances. [11] Construction of electrostatic interaction between carboxyl groups and various surfaces resulted in a catechol-chemistrybased hydrogel for the long-term adhesiveness. [12] Treatment by metal ions resulted in a hydrophobic surface that promoted formation of a water-resistant molecular bridge between the hydrogel surface and hydrophobic domains on the substrates, endowing the hydrogels prominent underwater-adhesion capability. [13] Similar adhesive hydrogel could also be achieved by dopamine-modified clay nanosheets. [14] An effective molecular structure design based on acid-ether hydrogen bonding and imine bonds was capable of accelerating hydrogel healing time to 30 min. [15] A dynamic borate bond in network enabled 100% cure of hydrogel in air. [16] Reversible metal-ligand coordination bonding interaction could also be used to construct self-healing hydrogel. [17] These protocols are efficient for the construction of functional hydrogels, yet still challenging to synchronously improve the mechanical strength, self-healing, and interfacial adhesion of a hydrogel, and especially, hard to endow the hydrogel with modular sensitivity to external pressure. Therefore, the development of a new class of protocol is still essential.Herein, we proposed an electrochemistry functionalization protocol, in which the functional improvements on hydrogels were achieved by the electrode reactions, and electrochemistrytriggered ionic and molecular migration. This protocol was capable of enabling the function improvements of the hydrogel in mechanical strength, interfacial adhesion, and self-healing. In the meantime, it allowed generation of various patterns on the hydrogel surface, and endowed the hydrogel modular sensitivity to external pressure. The functional improvements Hydrogels have demonstrated great potential in biomedical and engineering areas. To improve the physical performance, development of efficient physical/chemical protocols is essential. Herein, an electrochemistry functionalization strategy that is capable of enabling the functional improvements of hydrogel is reported. The electrochemistry functionalization is demonstrated on a hydrogel model of polyacrylamide (PAAm)@κ-carrageenan. The electrochemistry reaction generates metal ions (Fe 3+ ) that migrate and coordinate with the sulfate groups of κ-carrageenan resulting in the prominent function improvements. In comparison with untreated PAAm@κcarrageenan hydrogel, it c...