Microplate (MP) and microrod (MR)-type CoFe 2 O 4 /(Bi 3.25 Nd 0.65 Eu 0.10 )Ti 3 O 12 composite thin films were fabricated by a combination of reactive ion etching and metalorganic chemical vapor deposition. The effects of post-annealing temperature on the structural, magnetic, electrical, and magnetoelectric (ME) properties of the films were investigated. Based on the results, the optimal ferroelectric pillar structure to obtain a large ME voltage coefficient (α ME ) was determined. The electrical insulation properties for the films improved with increasing post-annealing temperature. On the other hand, magnetic and ferroelectric properties were degraded at high-temperature. Judging from the structural, magnetic, electric, and ME properties, the optimum post-annealing temperature was 700 °C. The shape of the ferroelectric layer had a significant influence on the ferroelectric properties and consequently on α ME . The MR shape exhibited a smaller clamping effect than the MP shape, producing a greater ME effect. The α ME for the MR-type film post-annealed at 700 °C was 5.5 mV cm −1 Oe −1 .