Density-functional　with　generalized　gradient　approximation　(GGA)　for　the　exchange-correlation　potential　has　been　used　to　calculate　the　energetically　global-minimum　geometries　and　electronic　states　of　NinAl　(n　=　2-8)　neutral　clusters.　Our　calculations　predict　the　existence　of　a　number　of　previously　unknown　isomers.　All　structures　may　be　derived　from　a　substitution　of　a　Ni　atom　at　marginal　positions　by　an　Al　atom　in　the　Nin+1　cluster.　Aluminum　atom　remains　on　the　surface　of　the　geometrical　configurations.　Moreover,　these　species　prefer　to　adopt　three-dimensional　(3D)　spacial　forms　at　the　smaller　number　of　nickel　atoms　compared　with　the　pure　Nin+1　(n　＞=　3)　configuration.　Atomization　energies　per　atom　for　NinAl　(n　=　2-8)　have　the　same　trend　as　the　binding　energies　per　atom　for　Ni-n　(n　=　3-9).　The　stabilization　energies　reveal　that　Ni5Al　is　the　relatively　most　stable　in　this　series,　in　comparison　with　the　magnetic　moment　of　pure　metal　nickel　(0.6　mu(B)),　the　average　magnetic　moment　of　Ni　atom　increases　in　Ni-Al　clusters　except　the　Ni3Al.　Moreover,　except　the　case　of　Ni5Al,　Ni　average　magnetic　moment　decreases　when　alloyed　with　Al　atoms　than　that　in　pure　Ni　clusters,　which　originate　the　effective　charge　transferring　from　Al　to　Ni　atoms.　(C)　2009　Wiley　Periodicals,　Inc.　Int　J　Quantum　Chem　110:　1368-1375,　2010