The development of methodologies for hard water treatment, i.e., the removal of calcium and magnesium ions, is highly demanded. In this sense, the use of ion-exchange materials stands out as a low cost-benefit strategy. Zeolites are well-known cation-exchangers, but that, due to their powder nature, present some drawbacks related to mass transfer and its recovery after use. To overcome such limitations, the preparation of hierarchical composites by adding a second class of pores appears as a viable alternative.[1] In this work, we present the development of chitosan-supported composites (CS₂-ZA₁-GA) containing zeolite NaA (ZA). This zeolite was synthesized via hydrothermal route using coal fly ashes as starting materials. The composites were prepared by dispersing the ZA in chitosan (CS) solution followed by gelation process. [2] The obtained materials were characterized using X-ray powder diffractometry, Fourier-transform infrared spectroscopy and scanning electron microscopy. The results indicate the successful preparation of porous composites containing zeolite NaA dispersed homogeneously in chitosan. Preliminary results of water softening showed that the composites present up to 60% of the zeolite NaA efficiency in the removal of Ca2+ ions from aqueous media.