In this paper, a facile and novel method was developed to fabricate high toughness and stiffness double network hydrogels made of ionical-linked natural hydrogel and synthetic hydrogel. The synthetic hydrogel network is formed firstly, and then the gel is soaked in the ionic solution to build second network to form double network hydrogel with high toughness and stiffness. Two different natural polymers, alginate and chitosan, are employed to build rigid and brittle network and poly(acrylamide) is used as soft network in double network hydrogel. The compressive strength of Calcium alginate/poly(acrylamide) double network hydrogels is increased twice than that of poly(acrylamide) single network hydrogels, and the Ca2+ ionically cross-linked alginate is the key to improve the compressive property of double network hydrogels as a sacrificial bond. However, the chitosan/poly(acrylamide) double network hydrogels exhibit no enhancement of compressive strength comparing to poly(acrylamide) single network hydrogels.