The high-resolution infrared spectra of the ν1 + ν3 (2CH) band of the Ar-C2H2 complex has been recorded from 6544 to 6566 cm(-1). The previously reported K(a) = 1 ← 0, 2 ← 1, and 0 ← 1 subbands were observed and the K(a) = 1 ← 2, 2 ← 3, and 3 ← 2 subbands were assigned for the first time. The intermolecular potential energy surface of this complex has been calculated ab initio and optimized by fitting the new high-resolution data. Refined intermolecular potential energy surfaces have been obtained for the ground vibrational state and for the excited v1 = v3 = 1 stretching state. For the former state, the results of the analysis are satisfactory and the microwave transitions of the complex are reproduced with a root-mean-square deviation of 5 MHz. For the latter state, systematic discrepancies arise in the analysis.