The adsorption and decomposition of NO have been investigated by using density functional theory method at the generalized gradient approximation level. We have performed calculations on adsorption energies and structures of NO on Ni(211) and Pd(211) surfaces with full-geometry optimization and compared them with the experimental data. The most favorite adsorption on both surfaces occurs at the bridge site parallel to step edge (sb), while the energy difference from the second favorite site of a threefold hollow site near step edge is less than 0.1 eV. Decomposition pathways have been investigated with transition state search. The decomposition pathway, where NO leans toward the step, is most probable for both surfaces. The overall activation energy for decomposition is 0.39 and 1.26 eV for Ni(211) and Pd(211), respectively. The present results clearly show that the NO molecules on Pd(211) are less activated than those on Ni(211). We have studied also reorganization of NO on Pd(211) at higher coverages up to 1/3 ML (monolayer) [three NO molecules in a (3 x 1) unit cell]. The site occupation is not in a sequential manner as the NO coverage is increased, and a reorganization of NO adsorbates occurs (the NO molecule at sb becomes tilting up at higher coverage), which can interpret the experimental data of Yates and co-workers very well.