Dehumidification is vital for human health and environmental sustainability. However, traditional moisture adsorbents have the problems like low adsorption capacity, high regeneration energy consumption and negative impacts to environment. As a result, it is demanding to develop environmentally friendly adsorbents with desirable adsorption capacity and convenient regeneration. Herein, a Linde type A zeolite@Mg-Al layered double hydroxides (LTA@LDH) with core-shell structure is synthesized by a facile in-situ co-precipitation method and used for indoor dehumidification. The LTA@LDH with hierarchically porous structure presents advantageous synergism of micro-mesopores, and exhibits a better adsorption and desorption performance than the pure LTA. The whole water uptake capacity of LTA@LDH is 0.339 g.g- 1 in relative humidity 95 % & 30 degrees C, much higher than that of pure LTA (0.248 g.g(-1)). The desorption activated energy of LTA@LDH is 53.92 kJ.mol(-1), nearly half of pure LTA (88.63 kJ.mol(-1)), indicating its superior desorption performance. The adsorption activity of LTA@LDH remains unchanged after fifteen consecutive adsorption-regeneration cycles. Based on various characterizations, a three-stage dehumidification model of LTA@LDH was proposed to reveal its unique sorption behaviors: (1) capillary condensation mainly in LTA's micropores; (2) mono-layer order water absorbed in LDH's mesopores; and (3) multi-layer water absorbed in LDH's mesopores. This work provides a new approach to design and develop zeolite-based adsorbents by introducing LDH and designing unique core-shell structure.