Design of new multifunctional nanosystems to integrate diagnostic and therapeutic functions is a major area of interest in the field of nanobiotechnology and nanomedicine. In this study, application of a new magnetic multilayered nanobiohybrid system composed of magnetite nanoparticles, silica, and albumin as a theranostic agent was investigated. Once the clusters of magnetite nanoparticles were coated with a silica shell, bovine serum albumin was conjugated to the surface of activated amine-MS particles (BMS). Afterwards, a curcumin-loaded albumin shell was formed on BMS particles (CBBMS). The curcumin loading capacity and efficiency of the nanobiohybrid particles were 93 ± 6 (mg drug/g particles) and 24 ± 1.7 (wt%), respectively. A sustained release profile was observed for the curcumin in PBS which followed the first-order kinetic model. Cytotoxicity evaluation of CBBMS showed a striking reduced IC value (9.9 μM) in comparison to that of the free curcumin (16.2 μM), tested on SH-SY5Y cells using MTT assay. Finally, the in vitro relaxivity experiments indicated a high transverse relaxivity (r) of 369.7 mM s for the superparamagnetic nanobiohybrid particles in magnetic resonance imaging (MRI) tests. The obtained results in drug delivery and MRI tests recommend the as-prepared multilayered nanobiohybrid particles as an efficient and suitable system for theranostic applications.