Bentonite-based tablets offer multiple advantages over other types of formulated tablets, including being biocompatible and cost-effective, and they can be used to develop gel-like matrices that have potential for use in sustained-release formulations. Developing a high-load sustained-release formulation has been reported to be challenging; therefore, the aim of this study was to develop systematically bentonite-based sustained-release tablets for a high-load active agent (ibuprofen) and investigate their release kinetics. Ibuprofen-loaded tablets (800 mg) were prepared using wet and dry granulation followed by enteric coating of the tablets. Fourier-transform infrared spectroscopy, differential scanning calorimetry and X-ray powder diffraction were used to evaluate the compatibility of ibuprofen with bentonite. The results show that these tablets comply with compendial requirements. In addition, the release profile of the formulations reveals that the drug follows a non-Fickian release model. The present formulation demonstrates a new use of bentonite as a safe and cost-effective excipient with adequate binding and compaction for preparing sustained-release tablets.