On a Ru (0001) surface Cs and CO form a very well ordered (Cs+CO)-(2×2) compound layer whose structure was analyzed recently (Cs on-top, CO in threefold sites). Here we present a vibrational analysis of the same system using high-resolution electron energy loss spectroscopy (HREELS), thermal desorption spectroscopy (TDS), and low-energy electron diffraction (LEED). The bonding of CO to Ru is both local and nonlocal. Two (C-O) stretch frequencies are observed depending on whether there are one or two CO molecules in the 2×2 cell. They change in energy between 155 and 204meV depending on CO coverage θCO. Setting θmax CO=1.0, the evolution of the C-O stretch intensities indicates that up to θCO=0.22 the 1-CO-(2×2) phase is formed exclusively implying some mobility of the Cs layer. For θCO.0.22 the 2-CO-(2×2) phase grows additionally until at θCO=1.0 only the 2-CO-(2×2) phase is found. Two Ru-CO stretch modes are observed for the first time and are assigned to adsorption in the hcp and fcc hollow sites within the 2×2 unit cell. They are very weak in intensity which is attributed to the threefold-hollow site and some screening in the 2D compound. With CO adsorption a change of the electronic structure of the Cs adlayer is observed; the adlayer loses metallicity and the Cs-Ru stretch becomes visible. Strong changes of the Cs-Ru stretch energies are observed with CO coverage.