  Grain boundaries control a wide variety of bulk properties in polycrystalline
materials, so simulation methods like density functional theory are routinely
used to study their structure-property relationships. A standard practice for
such simulations is to use compact, high-symmetry (coincident site lattice)
boundaries as representatives of the much more complex polycrystalline grain
boundaries. In this letter, we question this practice by quantitatively
comparing the spectra of atomic sites and properties amongst grain boundaries.
We show, using solute segregation as an example property, that highly symmetric
tilt boundaries (with {\Sigma} values less than 10) will fail to capture
polycrystalline grain boundary environments, and thus lead to incorrect
quantitative and qualitative insights into their behavior.
