All the possible geometrical structures of PtnNim(n+m=6,n、m≠0)clusters are optimized with a hybrid Density functional theory (B3LYP) at Lanl2dz level.For the ground state structures,the energy，thermodynamic properties，Nucleus Independent Chemical Shifts (NICS)，spectrum and polarizability are studied.The calculated results show that:the ground state structures of PtNi5,Pt2Ni4 and Pt3Ni3 clusters are quadrangular bi-pyramid,and Pt4Ni2 and Pt5Ni clusters are triangular bi-pyramid with hat and triangular pyramid with quadrilateral,respectively.From the point of view of thermodynamics,PtnNim clusters are stable because of the negative enthalpy of formation; the positive NICS of PtNi5 clusters show anti-aromaticity,the negative NICS of Pt2Ni4 and Pt5Ni clusters show aromaticity.The number of the IR absorption peak of Pt3Ni3 is the most.The IR and Raman absorption peak of PtNi5 ,IR of Pt2Ni4,Raman of Pt3Ni3 and Pt4Ni2 have only one.The absorption peak of Pt5Ni appears in the bigger frequencies only,and is zero almost in the small frequencies.