The near-infrared spectrum of Titan, Saturn's largest moon and one of the Cassini/Huygens' space mission primary targets, covers the 0.8 to 5 micron region in which it shows several weak CH4 absorption regions, and in particular one centered near 2.75 micron. Due to the interference of telluric absorption, only part of this window region (2.9–3.1 É m) has previously been observed from the ground [Noll, K.S., Geballe, T.R., Knacke, R., Pendleton, F., Yvonne, J., 1996. Icarus 124, 625–631; Griffith, C.A., Owen, T., Miller, G.A., Geballe, T., 1998. Nature 395, 575–578; Griffith, C.A., Owen, T., Geballe, T.R., Rayner, J., Rannou, P., 2003. Science 300, 628–630; Geballe, T.R., Kim, S.J., Noll, K.S., Griffith, C.A., 2003. Astrophys. J. 583, L39–L42]. We report here on the first spectroscopic observations of Titan covering the whole 2.4–4.9 É m region by two instruments on board the Infrared Space Observatory (ISO) in 1997. These observations show the 2.75-É m window in its complete extent for the first time. In this study we have also used a high-resolution Titan spectrum in the 2.9–3.6 É m region taken with the Keck [Geballe, T.R., Kim, S.J., Noll, K.S., Griffith, C.A., 2003. Astrophys. J. 583, L39–L42; Kim, S.J., Geballe, T.R., Noll, K.S., Courtin, R., 2005. Icarus 173, 522–532] to infer information on the atmospheric parameters (haze extinction, single scattering albedo, methane abundance, etc.) by fitting the methane bands with a detailed microphysical model of Titan's atmosphere (updated from Rannou, P., McKay, C.P., Lorenz, R.D., 2003. Planet. Space Sci. 51, 963–976). We have included in this study an updated version of a database for the CH4 absorption coefficients [STDS, Wenger, Ch., Champion, J.-P., 1998. J. Quant. Spectrosc. Radiat. Transfer 59, 471–480. See also http://www.u-bourgogne.fr/LPUB/TSM/sTDS.html for latest updates; Boudon, V., Champion, J.-P., Gabard, T., Loëte, M., Michelot, F., Pierre, G., Rotger, M., Wenger, Ch., Rey, M., 2004. J. Mol. Spectrosc. 228, 620–634]. For the atmosphere we find that (a) the haze extinction profile that best matches the data is one with higher (by 40%) extinction in the atmosphere with respect to Rannou et al. (2003) down to about 30 km where a complete cut-off occurs; (b) the methane mixing ratio at Titan's surface cannot exceed 3% on a disk-average basis, yielding a maximum CH4 column abundance of 2.27 km-am in Titan's atmosphere. From the derived surface albedo spectrum in the 2.7–3.08 micron region, we bring some constraints on Titan's surface composition. The albedo in the center of the methane window varies from 0.01 to 0.08. These values, compared to others reported in the other methane windows, show a strong compatibility with the water ice spectrum in the near-infrared. Without confirming its existence from this work alone, our data then appear to be compatible with water ice. A variety of other ices, such as CO2, NH3, tholin material or hydrocarbon liquid cannot be excluded from our data, but an additional unidentified component with a signature around 2.74 micron is required to satisfy the data.