The　interaction　of　cyanide　(CN)　with　different　sites　on　Ni(111)　surface　is　studied　by　using　density　functional　theory　(DFT).　Ni-19　cluster　is　used　to　simulate　the　surface.　The　present　calculations　show　that　the　end-on　bonded　(through　C　atom)　configuration　is　much　more　preferable　than　the　side-on　bonded　CN　or　other　configurations　on　the　same　adsorption　site.　For　all　adsorption　modes,　adsorption　energies　at　the　top,　bridge,　and　three-fold　sites　on　Ni(111)　are　comparable,　with　the　bridge　site　of　the　end-on　bonded　CN　(through　C　atom)　more　favorable　than　other　adsorption　sites.　CN　vibrational　frequencies　are　red-shifted　at　all　cases,　except　that　the　end-on　CN　bonded　(through　C　atom)　on　the　top　site　is　blue-shifted.　The　bonding　of　CN　on　the　Ni(111)　surface　is　largely　ionic.