A new 2D chiral cadmium coordination network [Cd(TCBA)2]·2EtO H(1) was prepared by the reaction of achiral angular asymmetric bridging ligand 2-((3,5-dimethyl-4H-1,2,4-triazol-4-yl)-carbamoyl)-benzoic acid(TCBA) with cadmium acetate, which was structurally characterized by IR, elemental analysis, thermogravimetric analysis and single-crystal X-ray diffraction. Complex 1 crystallizes in the chiral space group P21 and features a 2D chiral network consisting of two types of homo-chiral helices, which are further extended into a 3D chiral framework along the a-axis via hydrogen bonds. Moreover, powder second-order nonlinear optical(NLO) measurements reveal complex 1 has a modest second-harmonic-generation(SHG) efficiency at room temperature. A new 2D chiral cadmium coordination network [Cd (TCBA) 2] · 2EtO H (1) was prepared by the reaction of achiral angular asymmetric bridging ligand 2 - ((3,5-dimethyl-4H-1,2,4-triazol -4-yl) -carbamoyl) -benzoic acid (TCBA) with cadmium acetate, which was structurally characterized by IR, elemental analysis, thermogravimetric analysis and single-crystal X-ray diffraction. Complex 1 crystallizes in the chiral space group P21 and features a 2D chiral network consisting of two types of homo-chiral helices, which are further extended into a 3D chiral framework along the a-axis via hydrogen bonds. Moreover, powders second-order nonlinear optical (NLO) measurements reveal complex 1 has a modest second-harmonic-generation (SHG) efficiency at room temperature.