By bonding gold atoms to the magic number cluster (SiO2)(4)O2H4, two groups of Au-adsorbed shell-like clusters Au-n(SiO2)(4)O2H4-n (n = 1-4) and Au-n(SiO2)(4)O-2 (n = 5-8) were obtained, and their spectral properties were studied. The ground-state structures of these clusters were optimized by density functional theory, and the results show that in despite of the different numbers and types of the adsorbed Au atoms, the cluster core (SiO2)(4)O-2 of T-d point-group symmetry keeps almost unchanged. The absorption spectra were obtained by time-dependent density functional theory. From one group to the other, an extension of absorption wavelength from the UV-visible to the NIR region was observed, and in each group the absorption strengths vary linearly with the number of An atoms. These features indicate their advantages for exploring novel materials with easily controlled tunable optical properties. Furthermore, due to the weak electronic charge transfer between the Au atoms, the clusters containing Au-2 dimers, especially Au-8(SiO2)(4)O-2, absorb strongly NIR light at 900 similar to 1200 nm. Such strong absorption suggests potential applications of these shell-like clusters in tumor cells thermal therapy, like the gold-coated silica nanoshells with larger sizes.