We present a joint photoelectron imaging spectroscopic and theoretical investigation on the triatomic ZrC2- anion. Vibrationally resolved spectrum was acquired at 532 nm photon energy. Electron affinity for the neutral ZrC2 cluster was determined to be 1.60 +/- 0.07 eV. The CCSD(T) level of theory was used to explore the ground-state geometries and vibrational frequencies of the anionic and neutral ZrC2 clusters. Our vibrationally resolved photoelectron spectrum reveals two vibrational frequencies (564.6 and 1774.0 cm(-1)) of the neutral ZrC2 cluster, which correspond to the symmetric Zr-C-2 and C-C stretching modes, and these experimental findings are in good agreement with the calculated values. Additionally, the molecular orbitals and chemical bonding in the anionic and neutral ZrC2 clusters are also discussed to disclose the interaction between the transition metal atom (Zr) and C-2 unit.