The pairing of molecular magnets and nanomaterials couples top-down and bottom-up approaches to nanotechnology; facilitating a unique methodology to the controlled study of interfacial magnetic properties. Attaching Single-Molecule Magnets (SMMs) to "naked" gold nanoparticles is a novel method of exploring various avenues of magnetic nanotechnology, such as drug delivery, information storage, catalysis, and assembly of magnetic-nanostructural motifs. Herein we report the successful capping of laser ablation synthesized "naked" gold nanoparticles with a dinuclear dysprosium complex, while introducing new information regarding the changes in molecular magnetic properties upon surface attachment. We anticipate that this methodology in producing these magneto-plasmonic nanostructures not only provides answers to fundamental questions but also has the potential to provide new avenues to applications including information storage, multimodal imaging, biomedicine, and optoelectronics.