Herein, we report the molecular design and synthesis of two novel organic co-adsorbers DBA-1((Z)-2-cyano-3-(5-(4-(cyclohexa-1,5-dien-3-ynyl(phenyl)amino)phenyl)-1-hexyl-1H-indol-3-yl)acrylic acid) and (DBA-2) 5-((5-(4-(diphenylamino)phenyl)-1-hexyl-1H-indol-3-yl) methylene)pyrimidine-2,4,6 (1H,3H,5H)-trione with D-D-A (donor-donor-acceptor) architecture. We have combined the strong electron donating triphenylamine group with indole moiety attached to different acceptors/anchoring groups, as co-adsorbers for dye-sensitized solar cells and we present for the first time, the role of anchoring/acceptor unit on their co-adsorption properties. In this study, cyanoacetic acid and barbituric acid are employed as anchoring groups in the co-sensitizers DBA-1 and DBA-2, respectively. Their electrochemical and photo-physical properties along with molecular geometries, obtained from Density Functional Theory (DFT) are employed to vindicate the effect of co-sensitizer structures on photovoltaic properties of DSSCs. We have demonstrated that the co-sensitization effect is profoundly dependent upon the anchoring/acceptor unit in the co-adsorber molecule. Devices co-sensitized using DBA-1 and DBA-2 along with HD-2 (Ru-complex of 4, 4'-bis-(1,4-benzodioxan-5-yl-vinyl)-[2,2']bipyridine), displayed higher power conversion efficiencies (PCEs) than the device sensitized using only HD-2. In the present work, ruthenium based sensitizer, HD-2, has been chosen due to its better solar-to-power conversion efficiency and impressively higher photocurrent densities than that of standard N719. Among them, co-adsorber DBA-2, containing barbituric acid as the acceptor/anchoring group displays promising photovoltaic results and exhibited an enhanced efficiency of 8.06%. Further, good agreement between the calculated and experimental results showcase the precision of the energy functional and basis set utilized in this study. All these findings provide a deeper insight and better understanding into the intricacies involved in the design of superior co-sensitizers for development of highly efficient DSSCs. (C) 2016 Elsevier Ltd. All rights reserved.