Numerically optimized pulse sequences are promising candidates to address such challenges where both the nuclear spins show large anisotropic interactions. the Optimal Control (OC) for NMR pulse sequence development, which is a powerful tool and provides tailored pulse sequences for targeted systems. The control theory-based optimization algorithms (e.g., GRAPE(21)) have been implemented on simulation packages like SIMPSON and SPINACH . Nielsen and coworkers used OC-SIMPSON simulations to enable 2 H- 13 C CP in perdeuterated amino acids and proteins. Later, an analytical solution to this pulse sequence was determined RESPIRATION-CP to enhance its applicability beyond 2 H-13 C (25) to 13 C-15 N (26), 1 H-14 N ( ), and 1 H-31 P . OC simulations have also been used to enhance the sensitivity of multidimensional NMR experiments using Transverse mixing Optimal control Pulse (TROP) that enables the detection of phase-sensitive spectra with higher SNR. Optimal Control Double Cross Polarization (OC-DCP) and the recently introduced Optimal tm-SPICE sequence are examples of OC generated sequences for CP among spins with low gyromagnetic ratio (g). OC has also been used to design broad banded excitation pulses , efficient background signal suppressing sequence , and homonuclear decoupling sequence without a Bloch-Siegert shift . In this work, we introduce an Optimal Control (OC) generated pulse sequence for Optimal Polarization Transfer In Anisotropic Nuclear Spins (OPTIANS). The numerical simulation results indicate the higher efficiency in the simultaneous presence of 19 F CSA between 100 ppm to 250 ppm, and 7 Li quadrupolar interaction between 200 kHz to 340 kHz at magnetic fields of 9.4 T and 14.1 T. We used a model spin system consisting of four spins to represent all the major anisotropic interactions in practical cases. The resulting pulse sequence shows better efficiency and more robustness towards experimental imperfections such as power level mismatches compared to the standard CP method at 14.1 T. The experimental data supporting the simulated results are provided on a catalytically active multi-metal fluoride material. Since the 19 F-7 Li correlations are critical to gain insight into local structure and dynamics in many systems including catalysts, polymers, and battery materials, this new method has vast applicability that will further expand the scope of solid-state NMR in material research.