In this work soot formation was studied in laminar premixed flames of binary ethylene-benzene mixtures varying throughout the composition range from pure ethylene to pure benzene keeping constant the equivalence ratio (phi = 2) and obtaining a very similar maximum temperature (Tmax around 1750K). In such way, it was possible to study for the first time the effect of binary aliphatic-aromatic fuel mixtures composition on the sooting behavior in comparable combustion conditions. In-situ optical techniques (laser induced incandescence and fluorescence) and ex-situ particle size distribution (PSD) measured downstream of the flame front, as well as modeling by means of a multi-sectional method, were applied. PSD profiles showed that particles with sizes less than 10 nm decrease as benzene percentage in the feed mixture increases, disappearing for benzene percentages above 30%. Conversely, large aggregates grow towards sizes larger than 100 nm when benzene concentration is increased. A non-linear effect of the benzene content in the binary fuel mixture on soot particle concentration was observed by laser induced incandescence, and confirmed by the multi-sectional model. In particular soot formation was found to increase more than linear up to 50% then leveled off to reincrease linearly from 80% to 100%. On the contrary, particles smaller than 10 nm at the end of the flame rapidly decreased for benzene percentages larger than 30%. From reaction rate analysis, the formation of gas-phase polycyclic aromatic hydrocarbons (PAH) and high-molecular mass aromatics precursors was found to be significantly large already for fuel mixtures featured by low benzene amounts (from 10 up to 40-50%). The enhanced aromatic precursor formation, combined with the abundance of acetylene mainly coming from the dehydrogenation of ethylene as predominant component of the binary fuel mixture, appeared to be responsible for the non-linear effect of ethylene-benzene composition on particle formation, particularly significant up to 40-50% of benzene. This finding has a considerable importance as regards the exploitation of highly-aromatic fuels as well as to foresee the soot emission for effect of the aromatic presence in natural and synthetic fuels used in practical combustion systems. (C) 2018 The Authors. Published by Elsevier Inc. on behalf of The Combustion Institute.