The existing mold concept of fabricating magnetorheological elastomer (MRE) tends to encounter several flux issues due to magnetic flux losses inside the chamber. Therefore, this paper presents a new approach for enhancing particle alignment through MRE fabrication as a means to provide better rheological properties. A closed-loop mold, which is essentially a fully guided magnetic field inside the chamber, was designed in order to strengthen the magnetic flux during the curing process with the help of silicone oil (SO) plasticizers. The oil serves the purpose of softening the matrix. Scanning electron microscopy (SEM) was used to observe the surface morphology of the fabricated MRE samples. The field-dependent dynamic properties of the MREs were measured several ways using a rheometer, namely, strain sweep, frequency sweep, and magnetic field sweep. The analysis implied that the effectiveness of the MRE was associated with the use of the SO, and the closed-loop mold helped enhance the absolute modulus up to 0.8 MPa. The relative magnetorheological (MR) effects exhibited high values up to 646%. The high modulus properties offered by the MRE with SO are believed to be potentially useful in industry applications, particularly as vibration absorbers, which require a high range of stiffness.