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A series of single-phase T-structured NdSrCu_(1-x)Co_xO_(4-δ) with oxygen vacancies and T’-structured Sm_(1.8)Ce_(0.2)Cu_(1-x)Co_xO_(4-δ) (x:0-0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-progranuned desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCut_xCoxO4_b catalysts were of oxygen vacancies whereas the Sm_(1.8)Ce_(0.2)CU_(1-x)Co_xO_(4-δ) ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level,the oxygen vacancy density of NdSrCu_(1-x)Co_xO_(4-δ) decreased while the over-stoichiometric oxygen amount of Sm_(1.8)Ce_(0.2)CU_(1-x)Co_xO_(4-δ)increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO_(3.702) catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr~(-1), and 600-900℃, the catalytic activity of NO decomposition followed the order of NdSrCuO_(3.702)> NdSrCu_(0.8)Co_(0.2)O_(3.736) > NdSrCu_(0.6)Co_(0.4)O_(3.789) > Sm_(1.8)Ce_(0.2)Cu_(0.6)Co_(0.4)O_(4.187)> Sm_(1.8)Ce_(0.2)Cu_(0.8)Co_(0.2)O_(4.104)> Sm_(1.8)Ce_(0.2)CuO_(4.045), in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu~(3+)/Cu~(2+) redox ability of NdSrCu_(1-x)Co_xO_(4-δ) account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.