Attapulgite (denoted as APT, also called palygorskite) has been regarded as the green material in the "21st century world" and has attracted widespread attention due to its advantages of low cost, natural abundance, nontoxic nature, and environmental friendliness. However, the limited adsorption sites and surface charges of natural APT greatly hinder its application as an adsorbent in industrial fields. In this work, natural APT was modified with sodium humate (SA) via a facile one-step hydrothermal process to improve its adsorption capacity and systematically studied its ability to remove methylene blue (MB) from aqueous solutions. The effect of hydrothermal modification in the presence of SA on the microscopic structure, morphology, and physicochemical properties of APT was studied by field-emission scanning electron microscopy, Fourier transform infrared spectrometry, X-ray diffraction, and Brunauer-Emmett-Teller analyses. The adsorption properties of the modified APT toward MB were evaluated systematically. The results demonstrated that the modified APT has a high adsorption capacity of 227.27 mg/g and also shows a high removal rate up to 99.7% toward MB in a dye solution with an initial concentration of 150 mg/L, which was a 64.7% increase as compared to that of raw APT. The adsorption kinetics could be fitted to the pseudo-second-order model, while the adsorption isotherm could be well-described with the Langmuir model. It was concluded that electrostatic attraction, hydrogen-bonding interaction, and chemical association are the main driving force during the adsorption process.