Display omitted The transition metal complexes are playing the crucial role in advancement of modern chemical science. In the present study, we synthesized the Pd(II) complex Pd2 (C5H5F3N2)2(C5H4F3N2)2Cl2·3(C2H6O), 1 with 3-Methyl-5-(trifluoromethyl) pyrazoleligand. The complex 1 has been characterized by IR spectroscopy, elemental analysis and X-ray crystallography. The complex 1 crystallizes in triclinic space group P-1. Moreover, density functional theory (DFT) methods are successfully used not only to study the optical and nonlinear optical (NLO) properties of complex 1 but also to design its potential derivatives with Ni(II) and Pt(II) metals as complexes 2 and 3, respectively. The interaction energies are calculated for optimized complexes that are found to be −400, −524.41 and −504.16 kcal/mol for complexes 1, 2 and 3, respectively. The calculations for third-order nonlinear optical polarizability (γ) show that the average γ amplitudes for compounds 1, 2 and 3 are found to be 79.89 × 10−36, 71.24 × 10−36 and 102.09 × 10−36 esu, respectively. The γ amplitudes of compounds 1, 2 and 3 are about 4 times, 3 times and 5 times larger than that of para-nitroaniline (pNA), which is a prototype NLO molecule, respectively. The calculations of UV–Visible spectra show that the maximum absorption wavelength for complex 3 is around 260 nm with a significantly larger oscillator strength, which is about 4 times larger than the absorption spectra of complexes 1 and 2. The analysis of FMOs shows the ligand to metal intramolecular charge transfer (LMCT) process which might be the reason of larger NLO response properties in complex 3. Additionally, the calculations of global chemical reactivity descriptors indicate that the complexes are thermally and kinetically stable. Thus, we believe the present study will intrigue the scientific community to explore the designed complexes for optical and NLO applications.