Multiferroic composite materials operating under the principle of strain mediation across the interfaces separating different material boundaries address many limitations of single-phase magnetoelectric materials. Although significant research has been conducted to explore their responses relating to the topography and directionality of material polarization and magnetic loading, there remain unanswered questions regarding the long-term performance of these multiferroic structures. In this study, a multiferroic composite structure consisting of an inner Terfenol-D magnetostrictive cylinder and an outer lead zirconate titanate (PZT) piezoelectric cylinder was investigated. The composite was loaded over a 45-day period with an AC electric field (20 kV/m) at a near-resonant frequency (32.5 kHz) and a simultaneously applied DC magnetic field of 500 Oe. The long-term magnetoelectric and thermal responses were continuously monitored, and an extensive micrographic analysis of pretest and post-test states was performed using scanning electron microscopy (SEM). The extended characterization revealed a significant degradation of ≈30–50% of the magnetoelectric response, whereas SEM micrographs indicated a reduction in the bonding interface quality. The increase in temperature at the onset of loading was associated with the induced oscillatory piezoelectric strain and accounted for 28% of the strain energy loss over nearly one hour.