Palygorskite (Pal) is a natural abundant environment-friendly adsorbent that has shown high efficiency to decontaminate dye in water. However, the dye removal results in transformation of Pal to a very stable Maya Blue-like structure or waste Pal clay (WPal), which could not be easily regenerated by a commonly used desorption process. This paper presents a use of WPal as the precursor material to synthesize a highly-efficient mesoporous silicate/carbon composite adsorbent. The composite adsorbent has a large specific surface area (427.9 m²·g⁻¹), a high negative potential (−40.6 mV) and a mesoporous size (3.48 nm). This adsorbent shows almost complete removal of tetracycline (TC), crystal violet (CV) and methylene blue (MB) (initial concentration, 200 mg·L⁻¹) with the optimal adsorption capacities of 319.8 mg·g⁻¹, 244.4 mg·g⁻¹ and 281.7 mg·g⁻¹, respectively. The active -Si-O⁻ adsorption sites produced by the breaking of inert Si-O-Si (or M) bonds and the electrostatic interactions of negatively charged adsorbents to adsorbates play a major role in the adsorption process. Adsorption capacities of the developed composite are significantly higher than that of Pal, WPal and hydrothermally treated WPal (HWPal). Results demonstrate that the composite adsorbents have high potential in decontamination of organics in water efficiently.