In this work styrene-ethylene-butylene-styrene (SEBS) block copolymer based smart magnetorheological elastomeric (MREs) materials have been additively manufactured using solvent-cast 4D Printing (SC-4DP) technique. The effect of carbonyl iron powder (CIP) content on the particle distribution, particle–matrix adhesion, surface and layer morphology of the 4D Printed MRE sample was investigated. CIP particles were observed to be well embedded and dispersed up to 60 wt% content. However, at higher CIP content the tendency of the particles to agglomerate increased significantly. Furthermore, samples with CIP content ≥70 wt% showed poor particle–matrix adhesion and possessed inter-layer coalescence defects. Investigations were also performed to evaluate the magnetic properties of MREs at room temperature. Magnetorheological behaviour was studied to evaluate the effect of varying magnetic field on dynamic viscoelastic properties. Magnetorheological effect increased from ∼79 % to ∼211 % with an increase in CIP content. However, the particle–matrix adhesion also significantly affected the magnetorheological effect for higher CIP content samples. Magnetic actuation capability of flexible MRE samples was evaluated for gripper-based application. SC-4D Printed flexible grippers were able to successfully grip, lift, and drop both the soft deformable and rigid freeform profile objects in different media (air and sodium hydroxide solution) suggesting suitability for remotely actuated gripper-based applications.