Aluminum conductor steel-reinforced (ACSR) cables are typically used in overhead transmission lines, requiring stringent non-destructive testing owing to the severe conditions they face. Ultrasonic guided wave inspection provides promising online monitoring of the wire breakage of cables with the advantages of high sensitivity, long-range inspection, and full cross-sectional coverage. It is a very popular method to generate and receive guided waves using magnetostrictive and piezoelectric transducers. However, uniformly coupling the acoustic energy excited by transducers into multi-wire structures is always a challenge in the field application of guided waves. Long-term field application of piezoelectric transducers is limited due to the small coupling surface area, localized excitation, and couplant required. Conventional magnetostrictive transducers for steel strand inspection are based on the magnetostrictive effect of the material itself. Two factors affect the transducing performance of the transducers on ACSR cables. On one hand, there is a non-magnetostrictive effect in aluminum wires. On the other hand, the magnetostriction of the innermost steel wires is too weak to generate guided waves. The bias magnetic field is attenuated by the outer layers of aluminum wires. In this paper, an alternative sprayed magnetostrictive powder coating (SMPC) transducer was developed for guided wave generation and detection in ACSR cables. The Fe83Ga17 alloy powder with large magnetostriction was sprayed uniformly on the surfaces of certain sections of the outermost aluminum wires where the transducer would be installed. Experimental investigations were carried out to generate and receive the most commonly used L(0,1) guided waves for wire breakage detection at frequencies of 50 and 100 kHz. The results demonstrate that the discernable reflected waves of the cable end and an artificial defect of three-wire breakage (5.5% reduction in the cable’s cross-sectional area) were received by the transducer with SMPC, which was impossible for the transducer without SMPC. This method makes long-term and online monitoring of ACSR cables feasible due to the high coupling efficiency and good structural surface adaptability.