Hydrogel‐based materials are widely used in many fields, but most of them compared to tendons with the same water content do not exhibit high toughness, strength or fatigue resistance, which limits their application. The Hofmeister effect can adjust the mechanical properties of hydrogels by ions affecting the aggregation of polymer chains. Herein, we prepared a bioactivated hydrogel through simply mixing polyvinyl alcohol (PVA) and Na2CO3 aqueous solutions. PVA chains are aggregated by strong hydrogen bonds between CO32− and OH, at which stage the hydrogel is soft and easy to shape. Further salting out promotes the formation of crystal microphase of PVA chain, resulting in high mechanical strength and excellent toughness. The existence of Na2CO3 endow the hydrogel with conductivity, exhibits high and stable sensitivity in strain sensing, and could be used to monitor human actions. On the basis of this method, Ca2+ was added to prepare mineralized PVA hydrogels, which had high stability and long‐term swelling resistance in different ionic solutions. In vitro cell experiment, hydrogel had obvious effect of promoting bone cell proliferation and calcium deposition. This work provides a facile and feasible method for preparing bionic hydrogels with high strength, toughness, and adaptable shape.