To obtain reliable mass concentrations of solid particulate matter (PM) in the exhaust emissions from engines using optical instruments, it is essential that the solid PM used for instrument calibration has similar optical properties to the solid PM emitted from the engines being tested. The solid PM emitted from combustion engines is predominantly soot. The optical properties of soot are dictated by its chemical structure, size, and morphology. In this work, the chemical bond structure, primary-particle diameters, aggregate sizes, and morphological parameters of the soot emitted from two laboratory soot generators, widely used for calibrating instruments, are compared to those of soot emitted from three aircraft turbine engines using Raman spectroscopy and transmission electron microscopy. The Raman spectral properties, size, and morphology of soot emitted from aircraft engines are distinctly different from the properties of soot emitted from the soot generators operating under globally near-stoichiometric and fuel-rich conditions. These differences can be attributed to the variations in the size and orientation of the graphitic crystallites, amorphous-carbon content, amount of polyacetylene compounds, deposition of organic material, and extent of oxidation. Conversely, general agreement is observed between the chemical structure, size, and morphology of soot emitted from aircraft engines and the soot emitted from the soot generators operating at globally fuel-lean conditions. The findings of this investigation can be useful for identifying suitable soot particles for the calibration of instruments to measure the mass concentration of solid PM emissions from engines, and for other types of soot.