The ethene oligomerization performance of heterogeneous, Ni-based acid catalysts has been assessed by combining experimental measurements and Single-Event MicroKinetic (SEMK) modelling. In addition to the independently determined physisorption parameters, two catalyst descriptors, i. e., the ethene coordination enthalpy on the Ni-ion sites and the alkene protonation enthalpy on the acid sites, sufficed to adequately describe experimental data acquired on 1.8 wt% Ni-SiO2-Al2O3 and 4.9 wt% Ni-Beta zeolite. While Ni-sites ensure ethene dimerization, further alkylation, isomerization and cracking reactions occur on the acid sites. Unavoidably, alkylated species lead to product inhibition by hindering the accessibility of active Ni-ion sites for ethene. Very pronounced product physical adsorption was demonstrated to even result in reduced ethene conversion and, hence, catalyst activity. Through extensive reaction pathway analyses, guidelines for rational catalyst design for heterogeneous, Ni-based acid catalysts were proposed which are simulated to lead to selectivities of 60% towards 1alkenes, 50% towards gasoline and 25% towards propene. (C) 2017 The Author(s). Published by Elsevier Ltd.