Among various photovoltaic technologies available in the emerging market, dye-sensitized solar cells (DSSCs) are deemed as an effective, competitive solution to the increasing demand for high-efficiency PV devices. To move towards full commercialization, challenges remain in further improvement of device stability as well as reduction of material and manufacturing costs. This study aims at rational synthesis and photovoltaic characterization of two nanostructured electrode materials (i.e. SnO2 nanofibers and activated graphene nanoplatelets) for use as photoanode and counter electrode in dye-sensitized solar cells. The main objective is to explore the favorable charge transport features of SnO2 nanofiber network and simultaneously replace the high-priced conventional electrocatalytic nanomaterials (e.g. Pt nanoparticles) used in existing counter electrode of DSSCs. To achieve this objective, a multiphysics model of electrode kinetics was developed to optimize various design parameters and cell configurations. The porous hollow SnO2 nanofibers were successfully synthesized via a facile route consisting of electrospinning precursor polymer nanofibers, followed by controlled carbonization. The novel SnO2/TiO2 composite photoanode materials carry advantages of SnO2 nanofiber network (e.g. nanostructural continuity, high electron mobility) and TiO2 nanoparticles (e.g. high specific area), and therefore show excellent photovoltaic properties including improved short-circuit current and fill factors. In addition, hydrothermally activated graphene nanoplatelets (aGNP) were used as a catalytic counter electrode material to substitute for conventionally used platinum nanoparticles. Improved catalytic performance of aGNP electrode was achieved through increased surface area and better control of morphology. Dye-sensitized solar cells using these aGNP electrodes had power conversion efficiencies comparable to those using platinum nanoparticles with I-/I3- redox mediators. Moreover, a multiphysics model at the device level was developed to predict the power output characteristics of DSSC using different electrode materials. The developed model was validated by the experimental data acquired from lab-fabricated DSSCs. Further, parametric simulation was conducted to analyze the effect of series resistance, shunt resistance, interfacial overpotential, as well as difference between the conduction band and formal redox potentials on device performance. This model correlates the maximum power output of DSSC devices to various design and operating parameters, and it also provides insight into the working principles of newly designed devices.