Abstract The formation of support‐NCO and noble metal‐NCO groups on oxide supported noble metal catalysts and high area evaporated metal films during the NO/CO reaction was studied by FTIR spectroscopy. With SiO 2 and A1 2 O 3 as supports the results reported in the literature were essentially reproduced. With TiO 2 and ZrO 2 absorption bands in the region between 2000 and 2100 cm −1 were detected, which had not been described before. On evaporated metals NCO‐groups could be detected in situ. They are located at 2185 cm −1 for Pd and at 2170 cm −1 for Pt. Based on kinetic measurements the spillover of NCO‐groups from the noble metal to the support is proposed as a mechanism for support‐NCO formation. For this spillover a connection between support and noble metal is necessary, which is formed during hydrogen treatment at elevated temperatures. This connecting species could be a noble metal/support intermetallic phase, as Pd 3 Ti resp. Pt 3 T