Recently, photoresponsive nanoparticles have received significant attention because of their ability to provide spatial and temporal control over the drug release. In the present work, we report for the first time photoresponsive multifunctional magnetic nanoparticles (MNPs) fabricated using coumarin-based phototrigger and Fe/Si MNPs for controlled delivery of anticancer drug chlorambucil. Further, newly fabricated photoresponsive multifunctional MNPs were also explored for cell luminescence imaging. In vitro biological studies revealed that coumarin tethered Fe/Si MNPs of ~9 nm size efficiently delivered the anticancer drug chlorambucil into cancer cells and thereby improving the drug action to kill the cancer cells upon irradiation. Such multifunctional MNPs with strong fluorescence, good biocompatibility and efficient photocontrolled drug release ability will be of great benefit in the construction of light-activated multifunctional nano drug delivery systems.