We demonstrate the first application of a liquid-metal ion source for collinear laser spectroscopy in proof-of-principle measurements on naturally abundant In + . The superior beam quality, i.e., the actively stabilized current and energy of a beam with very low transverse emittance, allowed us to perform precision spectroscopy on the 5s 2 1 S0 → 5s5p 3 P1 intercombination transition in 115 In + , which is to our knowledge the slowest transition measured with collinear fluorescence laser spectroscopy so far. By applying collinear and anticollinear spectroscopy, we improved the center-ofgravity frequency νcg = 1 299 617 759. 3 (1.2) and the hyperfine constants A = 6957.19 (28) MHz and B = −443.7 (2.4) MHz by more than two orders of magnitude. A similar accuracy was reached for 113 In + in combination with literature data and the isotope shift between both naturally abundant isotopes was deduced to ν( 113 In) − ν( 115In) = 696.3 (3.1) MHz. Nuclear alignment induced by optical pumping in a preparation section of the ion beamline was demonstrated as a pump-andprobe approach to provide sharp features on top of the Doppler broadened resonance profile.