The detection performance of traditional infrared spectroscopy can be very limited in the case of molecular vibrational modes with low absorption cross-sections. On account of its electric field enhancement, plasmonic antenna can be combined with infrared spectroscopy to realize surface enhanced infrared detection and characterization of molecules. In this work, a super asymmetric cross antenna structure with tunable dual-frequency resonance and a high enhancement factor is designed. By systematically studying the transmission spectrum and charge distribution of this super asymmetric cross antenna structure, the physical origin of the dual-frequency resonance and its tunability are characterized in detail. In addition, in order to target desired molecular ensembles, the relationship between the resonance frequency and electric-field intensity of the two resonance modes and the parameters of structure and incident light are examined, yielding an enhancement factor close to 100 in the desired frequency region. Finally, the experimental results show that the proposed super asymmetric cross antenna structure can indeed generate dual-frequency resonances, agreeing reasonably with the theoretical results. It is believed that the super asymmetric cross antenna structure can be widely used to sensitively detect trace molecules, and in monolayered chemistry and bio-molecules, allowing their structures and dynamics to be studied using nonlinear infrared spectroscopy.