A rapid combustion process for the preparation of magnetic Mn0.5Co0.5Fe2O4 nanoparticles was introduced, which was composed of the preparation process of solution, combustion process and calcination process. The structure and properties of the as‐prepared product were investigated by X‐ray diffraction, scanning electron microscopy, transmission electron microscopy, and vibrating sample magnetometer. The results revealed that the volume of absolute alcohol and the calcination temperature were two key parameters for the preparation of Mn0.5Co0.5Fe2O4 nanoparticles. With the volume of absolute alcohol increasing from 15 to 100 mL, the particle size of Mn0.5Co0.5Fe2O4 nanoparticles calcined at 400°C for 2 h increased from 18 to 25 nm, and the saturation magnetization increased from 3.4 to 66.3 Am2/kg; while with the calcination temperature increasing from 400 to 700°C with 20 mL absolute alcohol, the particle size increased from 20 nm to 47 nm, the saturation magnetizations increased from 13.1 to 66.0 Am2/kg, and the specific surface area decreased from 102.99 to 0.13 m2/g. The adsorption characteristics of methyl blue (MB) onto Mn0.5Co0.5Fe2O4 nanoparticles at room temperature were investigated, and the regression equation was found in good agreement with the pseudo‐second‐order adsorption kinetics model with the initial MB concentrations of 50–200 mg/L; the adsorption equilibrium data of MB onto Mn0.5Co0.5Fe2O4 nanoparticles at room temperature were analyzed with Langmuir, Freundlich and Temkin models, and the adsorption isotherm was most effectively described by the Temkin model based on the value of the correlation coefficient (0.9931); the effect of pH on the adsorption of MB was examined, and the reusability of Mn0.5Co0.5Fe2O4 nanoparticles for adsorbing of MB revealed their excellent removal efficiency. © 2018 American Institute of Chemical Engineers Environ Prog, 38: S277–S287, 2019