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The fabrication of low-electrical-percolation-threshold polymer composites aims to reduce the weight fraction of the conductive nanomaterial necessary to achieve a given level of electrical resistivity of the composite. The present work aimed at preparing composites based on multiwalled carbon nanotubes (MWCNTs) and magnetite particles in a polyurethane (PU) matrix to study the effect on the electrical resistance of electrodes produced under magnetic fields. Composites with 1 wt.% of MWCNT, 1 wt.% of magnetite and combinations of both were prepared and analysed. The hybrid composites combined MWCNTs and magnetite at the weight ratios of 1:1; 1:1/6; 1:1/12; and 1:1/24. The results showed that MWCNTs were responsible for the electrical conductivity of the composites since the composites with 1 wt.% magnetite were non-conductive. Combining magnetite particles with MWCNTs reduces the electrical resistance of the composite. SQUID analysis showed that MWCNTs simultaneously exhibit ferromagnetism and diamagnetism, ferromagnetism being dominant at lower magnetic fields and diamagnetism being dominant at higher fields. Conversely, magnetite particles present a ferromagnetic response much stronger than MWCNTs. Finally, optical microscopy (OM) and X-ray micro computed tomography (micro CT) identified the interaction between particles and their location inside the composite. In conclusion, the combination of magnetite and MWCNTs in a polymer composite allows for the control of the location of these particles using an external magnetic field, decreasing the electrical resistance of the electrodes produced. By adding 1 wt.% of magnetite to 1 wt.% of MWCNT (1:1), the electric resistance of the composites decreased from 9 × 104 to 5 × 103 Ω. This approach significantly improved the reproducibility of the electrode’s fabrication process, enabling the development of a triboelectric sensor using a polyurethane (PU) composite and silicone rubber (SR). Finally, the method’s bearing was demonstrated by developing an automated robotic soft grip with tendon-driven actuation controlled by the triboelectric sensor. The results indicate that magnetic patterning is a versatile and low-cost approach to manufacturing sensors for soft robotics.