Aerobic oxidative condensation of benzylamine to N-benzylidenbenzilimine was carried out on new gold-based catalysts using as supports bimodal UVM-7-like mesoporous silica, containing Ni and Ce (or Sn) as oxide nanodomains partially embedded inside the mesoporous UVM-7 silica walls. These nano-domains acted as effective and stable inorganic anchors favoring the nucleation, growth and stability of supported gold particles. Following the Atrane method the stability of the oxide nanodomains during oxidation and thermal treatments was ensured. The catalysts were prepared in a two-step synthesis in which gold was incorporated through impregnation of previously synthesized bimodal porous silicas containing different heteroelements trapped by the silica mesostructure. The versatility of the preparative approach allowed high surface and accessibility of the mesoporous silica and also an easy and homogeneous inclusion of heteroelements in one pot. Aerobic oxidative condensation of benzylamine on these catalysts occurred selectively only with the formation of N-benzylidenbenzylamine. While the selectivity was total, the productivities (molproduct gcat-1 h-1) varied in a large range as a function of the catalysts composition (chemical composition and atomic ratios of the constitutive support elements). The catalytic behavior was merely controlled by the size of the gold particles, but the support is also exerting an effect. The best results were obtained on the mesoporous Au/Ce60-Ni10-UVM-7 catalyst having a 0.97(wt.%) gold content and preserving a relatively high surface (566 m2/g) and pore volume (0.91 cm3/g). The comparison with the individual or bicomponent catalysts led to the conclusion of a synergistic effect between the components. However, the main active specie of these catalysts was gold (without excluding the participation as promoter or co-catalysts of other oxidic phases containing Ni or/and Ce) and the method used for the preparation of these catalysts allowed an enough high dispersion of it to provide the determined activity.