Zeolite-like molecular sieves show high potential in solid desiccant dehumidification cooling systems. They are recognized for remarkable moisture adsorption capacity and regeneration performance, characterized by their S-shaped adsorption isotherms. As a new type of zeolite-like molecular sieves, AlPO4-LTA has been reported with superior equilibrium moisture uptake, but its dynamic dehumidification characteristics in practical dehumidification systems still lack. In this study, to explore the application potential of AlPO4-LTA, the material was synthesized through ionothermal method, followed by an examination of its features and moisture adsorption characteristics, focusing extensively on the dynamics of moisture adsorption and desorption. Moreover, the practical dehumidification characteristics of AlPO4-LTA coated dehumidifier were investigated by a validated mathematical model. Observations confirmed that the AlPO4-LTA possessed a uniform structure, a high specific surface area, and a narrow pore size distribution. The equilibrium moisture adsorption uptake can reach 0.42 kg·kg⁻¹ in adsorption isotherm of 30°C. The adsorption/desorption kinetics coefficients / of the AlPO4-LTA coatings determined by the linear driving force (LDF) model were on the magnitude of 0.001–0.01 s-1. Numerical results revealed the moisture removal capacity (MRC) and dehumidification coefficient of performance (DCOP) of AlPO4-LTA coated dehumidifier can reach 8.58 g·kg⁻¹ and 0.17 at regeneration temperature of 75°C, respectively, which were 1.8 and 1.1 times over those conventional AlPOs (including FAM-Z01 and EMM-8) coated dehumidifiers.