According to environmental concerns related to water pollution, this study aims to develop a novel hydrogel bead as a biocompatible and efficient adsorbent by integrating bacterial cellulose-activated carbon (BCAC) and montmorillonite (MT) in alginate hydrogel (ALG). The ionotropic gelation method was applied to the fabrication of BCAC/MT/ALG hydrogel beads. The BCAC/MT/ALG hydrogel bead exhibited significantly higher tensile strength, Young’s modulus, and thermal stability, with ~1.4 times higher adsorption uptake of methylene blue (MB) from aqueous solution as compared to the pristine ALG bead. The textural properties, including specific surface area and porosity, were beneficial to accommodate the size of cationic MB as the target molecule. This resulted in a remarkable MB adsorption uptake of 678.2 mg/g at pH 7 and 30 °C. The adsorption isotherm showed the best fit for the nonlinear Redlich-Peterson isotherm model. Experimental adsorption data were well-described by the pseudo-second order kinetic model, with R2 values reaching 0.997. In addition, the adsorbent bead demonstrated easy regeneration with high reusability with approximately 75% of MB removal after being used for six cycles. Therefore, BCAC/MT/ALG bead represents an eco-friendly, cost-effective, and highly efficient adsorbent for MB removal from water and could potentially be used for removal of a wide range of cationic dye pollutants from wastewater.