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We investigated whether the vertical roller mill can be efficiently used in the beneficiation of low-grade magnesite and whether it can improve upon the separation indices achieved by the ball mill. We conducted experiments involving the reverse flotation and positive flota-tion of low-grade magnesite to determine the optimum process parameters, and then performed closed-circuit beneficiation experiments using the vertical roller mill and ball mill. The results show that the optimum process parameters for the vertical roller mill are as follows: a grinding fineness of 81.6wt% of particles less than 0.074 mm, a dodecyl amine (DDA) dosage in magnesite reverse flotation of 100 g·t?1, and dosages of Na2CO3, (NaPO3)6, and NaOL in the positive flotation section of 1000, 100, and 1000 g·t?1, respectively. Compared with the ball mill, the use of the vertical roller mill in the beneficiation of low-grade magnesite resulted in a 1.28% increase in the concentrate grade of MgO and a 5.88% increase in the recovery of MgO. The results of our causation mechanism analysis show that a higher specific surface area and greater surface roughness are the main reasons for the better flotation performance of particles ground by the vertical roller mill in the beneficiation of low-grade magnesite.