wileyonlinelibrary.comadsorption and relatively high recombination rate via vacant sites that significantly restrict the photoconversion efficiency (PCE). Therefore, researchers are faced with the challenge of developing efficient suppression routes by designing this component with an efficient charge transport pathway. Although some approaches were reported to suppress the charge recombinations occurring at the TiO 2 /dye interface including the use of inorganic [3,4] as well as polymer-assisted materials, [5][6][7] there are still some practical limitations due to the poor light absorption, low surface area, and slow electron injection. To overcome these limitations, extensive research efforts are directed toward DSSC applications of functionalized photoanode electrodes with novel interface modifiers and toward the design of solar cells. An appropriate interface modifier can play the role of assisting charge separation and also effectively shield the unfavorable reactions which occur from the injected electrons in photoanode's conduction band (CB) to the I 3 − ions in electrolyte and/or to the holes in highest occupied molecular orbital (HOMO) level of the dye. [8] Among modifier layers, thin tunneling barrier (TTB) at TiO 2 /dye interface is one of the most efficient and feasible ways, because TTB material is preferred in such a way that its CB is more positive than that of TiO 2 to form an energy barrier which allows electron injection but hinders the recombination reactions as well as passivate the surface states known as the vacant sites.Since then, many groups have attempted to modify photoanode in this system using alternative materials. [5,9,10] However, it has still not been reached to the desired PCE due to lower electron transport efficiency and sensitizing ability, much faster recombination, and difficult bind with TiO 2 or dyes. Alternative to these molecules, deoxyribonucleic acid (DNA) molecules have attracted research interest as modifier and/or linker because of cost effectiveness/easy fabrication, absorption ability in UV region causing high intersystem quantum yield, and favorable energy levels (HOMO: −5.2 eV; LUMO: −1.1 eV) [11][12][13] to inject charge, its 3D double helix structure confines the entered photons, and these photons snatch electrons after each collision with DNA molecules. This double helix structure is also beneficial for sunlight utilization from all directions. [14] This paper firstly reports the effect of deoxyribonucleic acid (DNA) molecules extracted from chickpea and wheat plants on the injection/recombination of photogenerated electrons and sensitizing ability of dye-sensitized solar cells (DSSCs). These high-yield DNA molecules are applied as both linker bridging unit as well as thin tunneling barrier (TTB) at titanium dioxide (TiO 2 )/dye interface, to build up high-efficient DSSCs. With its favorable energy levels, effective linker bridging role, and double helix structure, bifunctional DNA modifier shows an efficient electron injection, suppressed charge recombinati...