This thesis presents the results of investigations of the synthesis, structure and physical properties of multiferroic materials. Multiferroics are materials in which two or all three of ferroelectricity, ferromagnetism and ferroelasticity occur in the same phase. Such materials have the potential applications of their parent materials, as well as new ones because of the interaction between the order parameters. The thesis is organized into four sections. Section 1 gives an overview of multiferroics, explaining the origin of mul-tiferroicity , occurrence of magnetoelectric coupling, their possible technological ap-plications and the challenges involved. Section 2 gives the scope of the investigations. The specific objectives of the present research on yttrium chromite, heavy rare earth chromites, solid solutions of yttrium chromite, rare earth manganites doped with alkaline earth metals, charge-ordered rare earth ferrites and indium manganite are outlined. Experimental aspects of the work carried out are discussed in section 3. It gives details of the experimental set up and the basic operation principles of various structural and physical characterizations of the materials prepared. In section 4, results of the investigations are discussed. Magnetic and di-electric properties of yttrium chromite (YCrO3), heavy rare earth chromites and YCr1-xMnxO3 are reported in section 4.1. These materials show canted antiferro-magnetic behavior below the Nel transition temperatures and dielectric transitions at high temperatures. Role of local non-centrosymmetry is discussed based on high-resolution neutron powder diffraction data. In 4.2 we discuss the results of charge-ordered rare earth ferrites which show good magnetoelectric effect. Magnetic, dielectric and magneto-dielectric properties of YCr1-xMnxO3 (Ln = rare earth) are discussed in 4.3. These materials show magneto-dielectric effect. In 4.4 we discuss the near normal incidence far infrared reflectivity spectra of a single crystal of TbMnO3, in the spectral range of 50cm−1 to 700 cm−1 from 10 K to 300 K. Finally in 4.5, magnetic and dielectric properties of bulk and thin films of indium manganite are discussed.