Herein, we have fabricated starch-borax double cross-linked network (DC) hydrogels with tough and self-healing properties using a one-pot method. The addition of borax significantly increased the storage modulus and loss modulus of these starch-borax DC hydrogels. The maximum compression stress (~288 kPa) of starch-borax DC hydrogels containing 5% borax was about ten times greater than that of a pure-starch hydrogel. The texture profile analysis values of the DC hydrogels-including hardness, springiness, cohesiveness, and adhesiveness-increased compared to pure-starch hydrogels. In addition, starch-borax DC hydrogels exhibited excellent self-healing and shape-recovery properties. These DC hydrogels, with a variety of excellent properties, have potential applications in agricultural, biomedical, and industrial fields.