We present a study of two spectral lines, Fe I 6173 Å and Ni I 6768 Å, that were candidates to be used in the Helioseismic and Magnetic Imager (HMI) for observing Doppler velocity and the vector magnetic field. The line profiles were studied using the Mt. Wilson Observatory, the Advanced Stokes Polarimeter and the Kitt Peak-McMath Pierce telescope and one-meter Fourier transform spectrometer atlas. Both Fe I and Ni I profiles have clean continua and no blends that threaten instrument performance. The Fe I line is 2% deeper, 15% narrower, and has a 6% smaller equivalent width than the Ni I line. The potential of each spectral line to recover pre-assigned solar conditions is tested using a least-squares minimization technique to fit Milne-Eddington models to tens of thousands of line profiles that have been sampled at five spectral positions across the line. Overall, the Fe I line has a better performance than the Ni I line for vector-magnetic-field retrieval. Specifically, the Fe I line is able to determine field strength, longitudinal and transverse flux four times more accurately than the Ni I line in active regions. Inclination and azimuthal angles can be recovered to ≈2° above 600 Mx cm-2 for Fe I and above 1000 Mx cm-2 for Ni I. Therefore, the Fe I line better determines the magnetic-field orientation in plage, whereas both lines provide good orientation determination in penumbrae and umbrae. We selected the Fe I spectral line for use in HMI due to its better performance for magnetic diagnostics while not sacrificing velocity information. The one exception to the better performance of the Fe I line arises when high field strengths combine with high velocities to move the spectral line beyond the effective sampling range. The higher g eff of Fe I means that its useful range of velocity values in regions of strong magnetic field is smaller than Ni I.