The influence of gemini surfactants (GSs) on the charging and aggregation features of anionic sulfate modified latex (SL) particles was investigated by light scattering techniques in aqueous dispersions. The GSs of short alkyl chains (2-4-2 and 4-4-4) resembled simple inert salts and aggregated the particles by charge screening. The adsorption of GSs of longer alkyl chains (8-4-8, 12-4-12, and 12-6-12) on SL led to charge neutralization and overcharging of the particles, giving rise to destabilization and restabilization of the dispersions, respectively. The comparison of the interfacial behavior of dimeric and the corresponding monomeric surfactants revealed that the former shows a more profound influence on the colloidal stability due to the presence of double positively charged head groups and hydrophobic tails, which is favorable to enhancing both electrostatic and hydrophobic particle-GS and GS-GS interactions at the interface. The different extent of the particle-GS interactions was responsible for the variation of the GS destabilization power, following the 2-4-2 < 4-4-4 < 8-4-8 < 12-4-12 order, while the length of the GS spacer did not affect the adsorption and aggregation processes. The valence of the background salts strongly influenced the stability of the SL-GS dispersions through altering the electrostatic interactions, which was more pronounced for multivalent counterions. These findings indicate that both electrostatic and hydrophobic effects play crucial roles in the adsorption of GSs on oppositely charged particles and in the corresponding aggregation mechanism. The major interparticle forces can be adjusted by changing the structure and concentration of the GSs and inorganic electrolytes present in the systems.