To remove toluene and methyl ethyl ketone (MEK) through adsorption, a honeycomb that is 60 cm in diameter and 40 cm in length was manufactured using ceramic paper as supporting material for adsorbents. Then, a mixture of Y type and ZSM-5 type zeolites with a ratio of 7:3 was impregnated on the surface of the honeycomb. By drying the impregnated material, the honeycomb adsorption rotor (HAR) was successfully manufactured. The amount of zeolites impregnated in the HAR was calculated to be 28 wt% and the peaks of the X-ray diffraction pattern of HAR were identical to those of the two kinds of zeolite powders. The small reduction in the BET surface area resulted from the reduction of mesopores while there was little reduction of micropores smaller than 100 nm, which plays a main role in the adsorptive separation of VOCs. Equilibrium adsorption for toluene and MEK of the HAR was measured 3.6 wt% and 3.3 wt%, respectively, at partial pressure of 0.2 mmHg. The experimental curves of equilibrium adsorption amount fitted well to the calculated curve by the Langmuir model; the interpretation of the breakthrough curve using material balances agreed with the test results. With 3 rph HAR rotation speed, 1.2 m/s face velocity, and 360 ppmv toluene and MEK inlet concentration, the rotary adsorption system showed average outlet concentrations of 18 ppmv and 14 ppmv, respectively, indicating removal efficiency was higher than 95%.