The flotation of diaspore and three kinds of silicate minerals, including kaolinite, illite and pyrophyllite, using an organosilicon cationic surfactant (TAS101) as collector and starch as depressant was investigated. The results show that both diaspore and aluminosilicate minerals float readily with organosilicon cationic collector TAS101 at pH values of 4 to 10. Starch has a strong depression effect for diaspore in the alkaline pH region but has little influence on the flotation of aluminosilicate minerals. It is possible to separate diaspore from aluminosilicate minerals using the organosilicon cationic collector and starch depressant. Further studies of bauxite ore flotation were also conducted, and the reverse flotation separation process was adopted. The concentrates with the mass ratio of Al2O3 to SiO2 of 9.58 and Al2O3 recovery of 83.34% are obtained from natural bauxite ore with the mass ratio of Al2O3 to SiO2 of 6.1 at pH value of 11 using the organosilicon cationic collector and starch depressant.