Smart structures with actuation function are desired for aerospace applications, including morphing airfoils, deployable structures and more. While shape memory alloys and piezoelectric ceramics and polymers are currently a popular smart material options for such applications, magnetoelastomers (MEs) can be uniquely actuated with application of non-contact magnetic field. Magnetoelastomers (MEs), composite materials made of magnetic particles and soft, non-magnetic matrix, can potentially contribute to such smart structures as a light-weight, smart material option with large strain change, fast response time (milliseconds) and anisotropic actuation properties. Other than aerospace applications, MEs, as soft actuators, have been investigated for flexible electronics, soft robotics, and biomedical applications. Anisotropic actuation properties of MEs can be controlled with particle organization within the elastomer. To provide this control, parametric studies on fabrication of MEs need to be performed. This study presents experimental work on nanoparticle organization within MEs using uniaxial, biaxial and triaxial magnetic fields and on the structure-property relationships of MEs. Iron oxide nanoparticles were used as a model nanofillers, and their surfaces were treated with silane coupling agent to improve dispersion and suspension within a polydimethylsiloxane (PDMS) elastomer. The fabricated MEs were inspected using microCT, and their anisotropic susceptibilities are being measured.