Adsorption of Chromium ions on Aluminium Pillared Interlayered Clays (Al-PILC) prepared from Bentonites originating from Pakistani sources of Peshawar and Samwal was investigated in a batch system. The raw clays were purified and chemically converted into Na-Bentonite. Pillaring procedure was performed on Na-Bentonite with pillaring oligomer solution to prepare Al-PILC. Both Raw and Al-PILC forms of Peshawar and Samwal clays were characterized by X-Ray Diffraction and Brunauer, Emmett, and Teller (BET) analysis before conducting adsorption studies. The effects of factors like adsorbent quantity, the concentration of adsorbate, pH and temperature were analyzed. Highly efficient adsorption of chromium ions in solution was achieved by Al-PILC. Based on the overall results of percentage removal of chromium ions in solution and in view of efficiency, simplicity, low cost, and reliability, Al-PILCs can provide a promising intervention for the elimination and control of environmental hazards associated with chromium pollution generated from leather industries in Pakistan.