Carbon microspheres have been synthesized by the hydrothermal method with fructose and a phosphoric acid solution at two different concentrations, which were used as precursors. The obtained materials were characterized by elemental analysis, X-ray powder diffraction (XRPD) analysis, scanning electron microscopy (SEM), nitrogen adsorption/desorption measurements, and Fourier transform infrared (FTIR) spectroscopy. Batch sorption experiments were performed to remove methylene blue (MB) from aqueous solutions by varying the initial concentration of MB (C₀) from 50 to 500 mg/dm³, contact period, solution pH value, and temperature. Prepared sorbents consisted of microsphere particles with diameters in the range of 0.6–2.7 µm. The synthetic route was found to govern the microporous–mesoporous structure and surface acidic functional groups of the final product. A phosphoric acid concentration of 40 wt.% gave carbon material with a specific surface area of 932 m²/g and a total pore volume of 0.43 cm³/g. It was found that the extent of MB sorption by the obtained carbon microspheres increased with initial dye concentration, contact time, and especially solution pH but slightly decreased with increasing temperature. Kinetic studies showed that the dye sorption process followed pseudo-second-order kinetics.