Vermiculite-based nano-adsorbent was successfully prepared via solution casting method from vermiculite that was first exfoliated by thermal shock followed by ultrasonic treatment. X-ray diffraction investigations showed that the combined effect of sonication and organo-modification led to extensive delamination of the vermiculite sheets. BET surface area measurements indicated flake thicknesses below 100 nm. Scanning electron microscopy images revealed that the organo-modification process of the vermiculite particles took place since the organo-modified sample presented a compact layer in its structure. Wastewater treatment performance evaluation of the synthesized vermiculite showed that the physicochemical and bacteriological properties improved significantly.It demonstrated that the material is efficient for wastewater treatment.