The magnetically levitated (Mag-Lev) centrifugal rotary blood pump (CRBP) with two-degrees-of-freedom active control is promising for safe and long-term support of circulation. In this study, Mag-Lev CRBP controllability and impeller behavior were studied in the simulated heart failure circulatory model. A pneumatically driven pulsatile blood pump (Medos VAD [ventricular assist device]-54 mL) was used to simulate the left ventricle (LV). The Mag-Lev CRBP was placed between the LV apex and aortic compliance tank simulating LV assistance. The impeller behavior in five axes (x, y, z, θ, and φ) was continuously monitored using five eddy current sensors. The signals of the x- and y-axes were used for feedback active control, while the behaviors of the other three axes were passively controlled by the permanent magnets. In the static mock circuit, the impeller movement was controlled to within ±10–±20 μm in the x- and y-axes, while in the pulsatile circuit, LV pulsation was modulated in the impeller movement with the amplitude being 2–22 μm. The amplitude of impeller movement measured at 1800 rpm with the simulated failing heart (peak LV pressure [LVP] = 70 mm Hg, mean aortic pressure [AoPmean] = 55 ± 20 mm Hg, aortic flow = 2.7 L/min) was 12.6 μm, while it increased to 19.2 μm with the recovered heart (peak LVP = 122 mm Hg, AoPmean = 100 ± 20 mm Hg, aortic flow = 3.9 L/min). The impeller repeated the reciprocating movement from the center of the pump toward the outlet port with LV pulsation. Angular rotation (θ, φ) was around ±0.002 rad without z-axis displacement. Power requirements ranged from 0.6 to 0.9 W. Five-axis impeller behavior and Mag-Lev controller stability were demonstrated in the pulsatile mock circuit. Noncontact drive and low power requirements were shown despite the effects of LV pulsation. The impeller position signals in the x- and y-axes reflected LV function. The Mag-Lev CRBP is effective not only for noncontact low power control of the impeller, but also for diagnosis of cardiac function noninvasively.