Four new heteroleptic ruthenium sensitizers [Ru(4,4′-carboxylic acid-2,2′-bipyridine)(L)(NCS)₂] (L = 5,5′-bis(4-octylthiophen-2-yl)-2,2′-bipyridine (1), 5,5′-bis(N,N-diphenyl-4-aminophenyl)-2,2′-bipyridine (2), 5,5′-bis(5-(N,N-diphenyl-4-aminophenyl)-thiophen-2-yl)-2,2′-bipyridine (3) and 5,5′-bis(4-octyl-5-(N,N-diphenyl-4-aminophenyl)-thiophen-2-yl)-2,2′-bipyridine (4)) were synthesized, characterized by physicochemical and computational methods, and utilized as photosensitizers in nanocrystalline dye-sensitized solar cells (DSSCs). The λ_max of the metal-to-ligand charge transfer (MLCT) absorption of these four ruthenium dyes (527 nm for 1, 535 nm for 2, 585 nm for 3 and 553 nm for 4) can be tuned by various structural modifications of the ancillary ligand and it was shown that increasing the conjugation length of such ligand reduces the energy as well as the molar absorption coefficient of the MLCT band. The maximum incident photon to current conversion efficiency (IPCE) of 41.4% at 550 nm, 38.6% at 480 nm, 39.4% at 470 nm and 31.1% at 480 nm for 1-, 2-, 3- and 4-sensitized solar cells were obtained. Respectable power conversion efficiencies of 3.00%, 2.51%, 2.00% and 2.03% were realized, respectively, when the sensitizers 1, 2, 3 and 4 were used in DSSCs under the standard air mass (AM) 1.5 sunlight illumination (versus 5.9% for standard N719).