A versatile method for decorating magnetic nanobeads (being composite materials from polymers and superparamagnetic nanoparticles) with silver nanoparticles of 3–6 nm size is presented. Control over the silver nanoparticle coverage at the nanobead surface is achieved by changing the reaction parameters. Moreover, the silver-decorated magnetic nanobeads (Ag-MNBs) are studied with respect to their in vitro cytotoxicity on two distinct tumour cell lineages under different parameters, i.e., dose, incubation time, magnetic field applied during the culturing, silver ion leakage, and colloidal stability. It is found that enhanced magnetically mediated cellular uptake and silver ion leakage from the Ag-MNBs surface are the main factors which affect the toxicity of the Ag-MNBs and allow the half-maximal inhibitory dose of silver to be reduced to only 32 μg mL−1. Furthermore, a synergic cytotoxicity induced by photo-activation of silver nanoparticles was also found.