Energy and environment concerns are among the huge challenges that the world is facing today. Encouraged by this realization is the evolution of the use of cleaner alternative energy. Dye-sensitized solar cells (DSCs) are potentially attractive candidates for the low cost manufacture which convert the solar energy into electricity. The work conducted during this thesis aimed at optimizing the DSC using three different strategies: Developing the new class of thiocyanate-free ruthenium Ru(II) for stable and efficient DSCs, the synthesis of osmium Os(II) sensitizers to harvest a larger fraction of the solar spectrum, and optimization of the device using the cobalt based electrolyte with Ru(II) sensitizers to enhance open-circuit voltage of DSC device. The first two chapters are the introduction to the photovoltaic devices, operation, and characterization techniques. In Chapter 3, we develop the new series class of thiocynate-free Ru(II) sensitizers by virtue of the bidentate and tridentate analogous pyridyl pyrazolate ancillary ligands. Chapter 4, we functionalize N749 sensitizer by incorporating the highly conjugated electron donating appendages. In Chapter 5, the design of Os(II) sensitizers will be an excellent option for expanding the spectral response well into the NIR region. Last chapter, it depicts that optimization of DSCs device with cobalt based electrolyte and the challenge of dye structure design. All strategies: ruthenium dyes, osmium sensitizers, cobalt based electrolyte, and device optimization are developed during this thesis make a valuable contribution to the development of high stability and efficiency DSCs, which try to pave the way to get opportunity for commercialization of DSCs in the future.