The synthesis of intrazeolite anchoring of [HRuCo3(CO)(9) (mu(2)-CO)(3)] involves the adsorption of metal carbonyl species into zeolite cages followed by reductive carbonylation under a mixed CO and H-2 atmosphere. The physicochemical characterization of the samples was based on a multianalytical approach, including Fourier transform-infrared, extended x-ray absorption fine structure spectroscopies, and CO/H-2 gas chemisorption. The research encomassed several key points as follows: (a) The generation process of bimetallic carbonyl clusters was considered to occur through the interaction of [Ru-Co], Co(CO)(4)(-) and Ru-I carbonyls, and conversion into [ HRuCo3(CO)(9)(mu(3)-CO)(3)] and further to [HRuCo3(CO)(9)(mu(2)-CO)(3)] isomer. (b) There is significant bimetallic interaction. (c) Internal and external confinement of [HRuCo3(CO)(9)(mu(2)-CO)(3)] were compared. (d) The intrazeolite anchoring of [RuCo3] carbonyl clusters shows a strong reaction with the extraframework Na+ alpha-cage cations, through involvement of the oxygen end of the bridging carbonyl ligands.