In the development of multifunctional devices, magnetoelectric (ME) multiferroic materials have gained an ever-increasing research interest in the field of science and technology. Magnetoelectric (ME) composites, which are an artificial combination of ferroelectric and ferromagnetic materials, show better coupling even above room temperature making them more practically important. In the present work we have investigated the eco-friendly ME composites in particulate (0-3 type) and bi-layered (2-2) forms using Ni-Zn ferrite as the ferrimagnetic phase and Ca, Sn substituted BaTiO₃ as the ferroelectric phase. Bilayered ME composite thin films, synthesized by PLD technique, with these individual phases was also carried out.