A mesoporous hybrid silicate microsphere with superior adsorption performance has been successfully synthesized by employing an “all-into-one” strategy and a simple one-pot hydrothermal process using naturally abundant low-grade red palygorskite (PAL) clay as raw material in the presence of nontoxic SiO₃²⁻ and Mg²⁺ ions. As is expected, both the PAL and associated minerals transformed into a new amorphous mesoporous hybrid silicate microsphere without using any additional pore-forming template. The mesoporous silicate microsphere shows a large pore size of 37.74 nm, high specific surface area of 489.81 m2/g (only 54.67 m²/g for raw PAL) and negative surface potential of −43.3 mV, and its maximum adsorption capabilities for Methylene bule (MB) and Crystal violet (CV) reach 407.95 mg/g and 397.22 mg/g, respectively. Meanwhile, 99.8% of MB (only 53% for raw PAL) and 99.7% of CV (only 43% for raw PAL) were sucessfully removed from 200 mg/L of initial dye solution by only using 1 g/L of the adsorbent. In addition, the spent adsorbent can be easily regenerated and repeatly reused for muptiple cycles. The study on adsorption mechanism revealed that electrostatic attraction, hydrogen bonding and chemical complexing interactions are the main factors contributed to the high dye adsorption.