In the past years, the use of highly sensitive silicon microelectromechanical cantilevers has been proposed as a tool to characterize the spin-crossover phenomenon by employing fast optical readout of the motion. In this work, FeII-based spin-crossover nanoparticles of the well-known [Fe(Htrz)2(trz)](BF4) complex wrapped with thin silica shells of different sizes will be studied by means of silicon microresonators. The silica shell will enhance its chemical stability, whereas the low thickness will allow a proper mechanical coupling between the cantilever and the spin-crossover core. To maximize the sensing of the spin-crossover phenomena, different cantilever geometries and flexural modes were employed. In addition, the experimental observations were also compared with COMSOL numerical simulations, which are in close agreement with them. The probe of spin-crossover phenomena with micro- and nanoelectromechanical actuators offers the possibility of preparing smart sensing memory devices near/above room temperature.