The aggregation of silanized glass spheres (75 +/- 5 mum diam) was studied experimentally at liquid-air (water-air, aqueous surfactant solution-air, and aqueous glycerol solution-air) interfaces from a kinetic point of view. The number the size, and the polydispersity of clusters was Investigated as a function of time. Particles having water contact angles of approximate to 30 degrees (lower hydrophobic sample) and approximate to 82 degrees (higher hydrophobic sample) were prepared and used in the aggregation experiments. In the early stage of aggregation the kinetics was found to be-of the second order. The-experiments revealed that the increasing particle hydrophobicity increased the rate constants in every case, which could be attributed to the increasing particle-particle attractions and the decreasing hydrodynamic resistance of particles (clusters) to motion. Moreover, the lower hydrophobicity of particles manifested itself in a more important polydispersity of clusters and an unexpected cross-over during the growth. The cluster-cluster aggregation was succeeded by a particle- (large) cluster aggregation after the first (initial) part of the growth. An off-lattice computer simulation of cluster-cluster aggregation, based on molecular dynamics, was also developed for the better understanding of the interfacial aggregation. The simulations supported well the conclusions derived from the real experiments, and gave an indispensable possibility for the study of the effect of single parameters on the complex phenomenon.