Hydrogels are wet and soft materials with rubber-like properties. The excellent biocompatibility and stimuli-responsiveness have made hydrogels excellent candidates in the field of materials science. However, most of the hydrogels are extremely soft (modulus of approximately 0.1 MPa) as compared to rubber materials; this greatly limits their application in the field of material engineering. In this study, an Al³⁺-reinforced carboxymethyl cellulose/polyacrylic acid hydrogel was first synthesized by a facile, visible-light-triggered, one-pot polymerization method. Subsequently, the as-prepared hydrogel was reinforced by evaporation-swelling (E-S) treatment to obtain a hydrogel (HM-Gel) with a 10-fold higher elastic modulus. This hydrogel exhibits a tensile strength of 1.26–1.74 MPa and an elastic modulus of 0.59–1.94 MPa. Moreover, the HM-Gel, with an excellent vibration absorption ability, can find applications in the field of industrial engineering and bioengineering.