Chiral Ni(II) coordination compounds with structures of [NiL(H2O)(3)] (1) and {[NiL(H2O)]center dot 0.5H(2)O}(n) (2) (H2L = thiazolidine 2,4-dicaboxlic acid) have been successfully synthesized by the reaction of Ni(CH3COO)(2)center dot 4H(2)O and H2L in aqueous solution at 25 and 80 degrees C, respectively. From the same procedure with polyvinylpyrrolidone (PVP) as a surfactant, another corresponding micrometer-scale Ni(II) coordination polymer, {[NiL(H2O)(2)]center dot H2O}(n) (3), has been obtained at both 25 and 80 degrees C, which shows a different structure (one-dimensional, ID) than both 1 (discrete molecule) and 2 (3D). The conversions of structures and conformations are directed by temperature and surfactant (PVP), as confirmed by powder and single-crystal X-ray diffraction. Circular Dichroism (CD) and Second Harmonic Generation (SHG) measurements of the products have been investigated as well; which indicate the potential applications of these products in chiral and nonlinear optical (NLO) areas.