Polydopamine-modified granule organo-attapulgite adsorbent (PDA-GOAT) was facilely prepared via a dip-coating approach. The samples were characterized by scanning electron microscopy, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. Surface area and pore size were calculated from the Brunauer–Emmett–Teller method by N2 adsorption–desorption isotherm. The adsorption behaviour of methylene blue (MB) onto PDA-GOAT was systematically investigated. The experimental data revealed that the adsorption process fitted well with the pseudo-second-order kinetics equation and the adsorption isotherm fitted better with the Langmuir model. Thermodynamic analyses illustrated that MB adsorption onto PDA-GOAT was a physisorption endothermic process. Importantly, PDA-GOAT can be regenerated by NaBH4 aqueous solution. The obtained results prove that PDA-GOAT can be a superior reusable adsorbent for the removal of MB from effluent.