The perovskite structure with general formula ABX3 shows its multidimensional nature in regards to correlations of crystal structures with electronic, magnetic, optical, and catalytic properties. Perovskites are utilized in a large range of applications due to their tremendous versatility. In this chapter, structure-properties correlations in oxide perovskite compounds ABO3 having several functional properties are presented. In particular, neutron and x-ray diffraction results are described to reveal a direct correlation of several important physical properties, such as magnetic, multiferroic, electronic (CMR), and SOFC electrodes with the crystal structures.