A ruthenium complex trans-[Ru(L)(NCS)2], L ) 4,4¢¢¢-di- tert-butyl-4¢,4¢¢-bis(carboxylic acid)-2,2¢:6¢,2¢¢:6¢¢,2¢¢¢- quaterpyridine (N886), was synthesized and characterized by spectroscopic and electrochemical methods. The absorption spectrum of the N886 complex shows metal-to-ligand charge-transfer transitions in the entire visible region and quasi-reversible oxidation and reduction potentials at E1/2 ) +0.38 and -1.92 V vs ferrocene, respectively. The electronic spectra of the N886 complex were calculated by density functional theory (DFT)-time-dependent DFT, which qualitatively reproduces the experimental absorption spectra for both the protonated and deprotonated species. From the analysis of the computed optical transitions of N886, we assign its absorption bands as mixed Ru/SCN-to-quaterpyridine charge-transfer transitions, which extend from the near-IR to the UV regions. The panchromatic response of the N886 complex renders it as a suitable sensitizer for solar energy conversion applications based on titanium dioxide mesoporous electrodes. The preliminary results using the N886 complex as a sensitizer in a dye-sensitized solar cell, with an electrolyte containing 0.60 M butylmethylimidazolium iodide, 0.03 M I2, and 0.50 M tert-butylpyridine in a mixture of acetonitrile and valeronitrile (volume ratio 1:1), show 40% incident photonto- current efficiencies, yielding under standard AM 1.5 sunlight a short-circuit photocurrent density of 11.8 ± 0.2 mA/cm2, an open-circuit voltage of 680 ± 30 mV, and a fill factor of 0.73 ± 0.03, corresponding to an overall conversion efficiency of 5.85%.