A double-mesoporous nanosystem was synthesized for treating as well as imaging cancer cells by using a simple and mild method. The mesoporous platinum (Pt) nanoparticles acting as a core show excellent photothermal effect under illumination with an 808 nm near infrared (NIR) laser. The mesoporous silica linked with a lanthanide (Gd) complex acting as a shell displays potential applications as a contrast agent for magnetic resonance imaging (MRI). The final mPt@mSiO2-GdDTPA nanosystems exhibit good biocompatibility in vitro and in vivo, when investigated by methyl thiazolyl tetrazolium assay and histological and serum biochemistry analysis. The investigation of the photothermal effect shows that the mPt@mSiO2-GdDTPA nanosystems exhibit an excellent photothermal therapy effect on HeLa cells and tumor-bearing mice. As theranostic agents, the nanosystems display a higher r1 value than the medical contrast agent magnevist and were successfully applied to in vivo MRI of Kunming mice. Therefore, the first systematic study on the photothermal effect of nanosystems based on mesoporous Pt nanoparticles does encourage the potential applications of metal nanoparticles and hybrid nanocomposites for cancer bioimaging and therapy.