Diatomic ZrFe has been spectroscopically investigated for the first time, with the optical spectrum recorded in the range from 13890 cm(-1) to 18870 cm(-1). In the region from 13890 to 17500 cm(-1), a single exceptionally weak vibrational progression is found. Band origins, excited state vibrational frequencies and anharmonicities, excited state lifetimes, and the ground state vibrational interval, Delta G(1/2)'', are reported for the five most abundant isotopomers. For the most abundant species, (ZrFe)-Zr-90-Fe-56 (47.2%), these values are: T-0 = 13931.9(1.2) cm(-1), omega(e)' = 325.05(54) cm(-1), omega(e)'x(e)', = 1.589(40) cm(-1), and Delta G(1/2)'' = 452.2 cm(-1). Rotationally resolved studies have revealed ground and excited state rotational constants and Omega values, bond lengths and rotation-vibration constants, giving B-0 '' = 0.138786(30) cm(-1) and r(0)'' = 1.87685(20) angstrom for (ZrFe)-Zr-90-Fe-56. The ground state and all observed excited states have Omega = 0. On the basis of the short bond length, the ground state of ZrFe is assigned as a nominally sextuply bonded (1)Sigma(+) (Omega = 0(+)) state deriving from the 1 sigma(2)1 pi(4)2 sigma(2)1 delta(4) electronic configuration. Above 18000 cm(-1), the spectrum becomes much more intense and congested, indicating the onset of electronically allowed transitions in this region.