Soot formation is experimentally and numerically investigated in laminar counterflow diffusion flames burning ethylene and three typical gasoline surrogate components; n-heptane, iso-octane, and toluene. Laser-induced incandescence and a light extinction technique are employed to determine the soot volume fraction within the well-controlled region of the burner. The experiments are performed across a wide range of strain rates and stoichiometric mixture fractions. From the experimental data, sensitivities of soot formation on strain rate and stoichiometric mixture fraction are derived for each fuel. The fuels show significantly different sensitivities. For iso-octane and n-heptane, a higher sensitivity of soot production on the strain rate is observed as compared to ethylene and toluene. Moreover, the sensitivities of soot formation on the strain rate increase with increasing stoichiometric mixture fraction. One-dimensional simulations of the flames investigated experimentally were performed using two different detailed chemical kinetic mechanisms, detailed chemical soot models, and the hybrid method of moments as well as a discrete sectional method to describe soot dynamics. The models are capable of predicting the soot volume fraction of the ethylene flames with remarkable accuracy, whereas for the gasoline surrogate components, the overall soot volume fractions are overpredicted for all tested models. In iso-octane flames, soot nucleation and PAH condensation rates are particularly enhanced. A reaction pathway analysis shows that in ethylene flames, the formation of benzene mostly originates from acetylene, while for iso-octane, large amounts of iso-butenyl form propyne, propargyl, and then benzene. (C) 2019 The Combustion Institute. Published by Elsevier Inc. All rights reserved.