Controlling the polarization states of transmit waveforms can improve the performance of radar systems, especially for main lobe jamming suppression applications. In this paper, we consider the design of optimal transmit polarizations for deceptive jamming suppression in the main lobe using a game theory framework. We propose a co-located polarization multiple-input multiple-output (MIMO) radar system that combines the advantages of MIMO radar and those offered by optimally choosing the transmit polarization to improve the jamming suppression performance. In the polarization MIMO radar, polarization diversity is employed in the transmit array, and 2-D vector sensors are adopted in the receive array to separately measure the horizontal and vertical components of the received signals. Furthermore, based on the concepts and advantages of game theory, we formulate a polarization design problem for this radar system as a twoplayer zero-sum (TPZS) game between the radar and jammers. Additionally, we propose two design methods for different cases: a unilateral game for dumb jammers, and a strategic game for smart jammers. The optimal strategy and Nash equilibrium solution for two cases are presented. The simulation results demonstrate that jamming can be effectively suppressed with the proposed radar configuration and that improved jamming suppression performance can be achieved when the transmit polarization scheme is designed using the game theory approach.