In this research, to optimize the surface of the photoanode, two different types of surface coatings were used and their effects on the photovoltaic parameters were investigated. Also, to compare the two different electrolytic systems based on liquid and gel-state electrolyte, the novel magnetic core-shell nanocellulose/titanium chloride (Fe3O4@)NCs/TiCl) nanocomposite was introduced into a polymeric system as a nanofiller to decrease the crystallinity of the polymer and enhance the diffusion of triiodide ions in quasisolid-state dye-sensitized solar cells (QS-DSSCs). For this purpose, Fe3O4@)NCs/TiCl was synthesized by coprecipitation of Fe3+ and Fe2+ ions in the presence of nanocellulose and then used as magnetic support for bonding TiCl4 to prepare QS-DSSCs. Containing a 10.0 wt% magnetic nanocomposite, it displayed a higher apparent diffusion coefficient (D-app) for I-3(-) ions (4.10 x 10(-6) cm(2)/s) than the gel polymeric electrolyte (GPE) did (1.35 x 10(-6) cm(2)/s). GPEs were characterized using various techniques including current density-voltage curves, AC impedance measurements, and linear sweep voltammetry (LSV). The photovoltaic values for the short-circuit current density (J(sc)), open-circuit voltage (V-OC), and fill factor (FF) and the energy conversion efficiency (eta) of the novel Fe3O4@NCs/TiCl nanocomposite-based QS-DSSCs were 14.90 mA cm(-2), 0.757 V, 64%, and 7.22%, respectively.