Silicate clay materials are promising natural adsorbents with abundant, low cost, stable, and ecofriendly advantages, but the limited adsorption capacity restricts their applications in many fields. Herein, palygorskite (PAL) was facilely activated with alkali to enhance its adsorptive removal capability for methylene blue (MB). The effects of alkali activation on the microstructure, physicochemical, and adsorption properties of PAL for MB were intensively investigated. It was found that the moderate alkali activation can partially remove the metal cations (i.e., Al³⁺, Mg²⁺) and Si in the crystal backbone of PAL by which new Badsorption sites^ were created and the surface negative charges increased. The adsorption capacity and rate of PAL for MB were evidently enhanced due to the effective activation. The adsorption isotherms were described by Freundlich isotherm model very well, and the adsorption kinetics can be accurately presented by a pseudo-second-order model. It can be inferred from the fitting results that the overall adsorption process was controlled by external mass transfer and intra-particle diffusion (the dominant role). The multiple adsorption interactions (hydrogen bonding, electrostatic interactions, mesopore filling, and complexing) were turned out to be the dominant factors to improve the adsorption properties. It was revealed that the activated PAL could be used as a potential adsorption candidate for environmental applications.