This thesis presents novel solutions for the fabrication of functional magnetoresponsive systems, with a focus on the development of magnetic composites as sensors and actuators. Currently, there is a need for multifunctional mechanically flexible materials that can be easily processed into functional devices that respond to a wide range of physical stimuli, including magnetic fields. These characteristics aim for lightweight, and imperceptible systems that help us to interact with technology and with each other without the need for a bulky gadget. Typically, magnetically responsive devices are constructed using materials that do not necessarily possess flexible properties; so magnetosensitive composites with tailored magnetic, conductive, and flexible properties arising from the combination of their constituents were implemented. Here, it is described the use of these composites as printable sensors for magnetic field detection, with a focus on interactivity, safety, and holographic-like applications. A dedicated selection of materials and fabrication methods allowed to obtain stretchable, transparent, or self-healing properties, as well as explore their possibilities for printing them over large-area or even 3D printing. Additionally, it is shown the use of these magnetoresponsive composites as actuators, demonstrating their potential use in magnetic soft robotics by laminating magnetically sensitive devices that give them a sense of motion. Such applications become more technically accessible after the proposition of measurement strategies that remove artifacts in the magnetic signal coming from mechanical deformations. This thesis addressed several of the challenges related to cost, fabrication, and integration in magnetoresponsive composites, and is expected that related research might develop through multifunctional composites that sense more than magnetic fields.