Due to the influences of inductance, resistance, and the third harmonic back electromotive force (back EMF), there is the third harmonic current in five-phase permanent magnet synchronous motors (PMSMs) with model predictive torque control (MPTC) based on finite control set (FCS). To suppress the third harmonic current while improving operating performance, a novel virtual-FCS-based MPTC strategy with harmonic current suppression was proposed in this article. The novelty of the proposed strategy is the development of new groups of FCSs and the concept of virtual FCS based on closed-loop regulation of harmonic current. Consequently, the double closed-loop control is simultaneously achieved in two orthogonal subspaces by the FCS. Thus, without the harmonic current term of cost function, the third harmonic current suppression is enhanced and the total harmonic distortion (THD) of phase current is reduced. In addition, lower switching frequency, higher efficiency, good steady-state performance, and high dynamic torque response can be obtained without heavy computation burden. Simulation and experimental results are presented to validate the effectiveness of the proposed method.