High water consumption during irrigation is one of the main problems in agriculture. The preparation of a material that prolongs the water retention capacity of the soil is important. This article aimed to prepare superabsorbent hydrogels by the complexation of chitosan (CHI), with high degree of deacetylation (DD), and carboxymethylcellulose (CMC), with high degree of substitution (SD). Different parameters (concentration and polymeric solutions addition order, polysaccharides’ ratio, pH) were studied. Morphology, thermal stability, chemical composition, mechanical strength, and swelling kinetics of hydrogels in water were evaluated. A hydrogel formation mechanism was discussed and proposed. Results showed that most samples prepared at acid pH disintegrated during swelling test. The morphology of the hydrogels varied with the pH. It was obtained superabsorbent hydrogels (swelling > 400%) based on CMC (SD = 2.23) and CHI (DD = 92%), at basic pH, with good compression strength, and applicable as soil conditioner. The best sample was the one prepared with CMC:CHI = 1:2, polymeric solutions 1.5% m/v and pH 8.