Cross-polarization is one of the most used methods in solid-state NMR to obtain local structural and dynamic information. The limitations on the CP efficiency posed by the large CSA and quadrupolar coupling have restricted its applications in material research. A vast number of materials contain NMR isotopes with spin>1/2 such as 6/7 Li, 23 Na, 27 Al, etc., and spin-1/2 isotopes, such as 19 F, 195 Pt, 207 Pb, etc., that have large CSA. Hence an efficient CP method for such NMR isotopes is essential to expand the scope of the technique to a broader category of materials. Here, we used optimal control simulations to design a new pulse sequence to handle such cases. The target spin system was 19 F- 7 Li, but the proposed method is valid for a larger set of spin-pairs including 19 F-23 Na, 19 F-27 Al, 19 F-13 C, etc. The simulated polarization transfer curves for these cases are shown in the SI Figure . The OPTIANS shows the transient oscillations in the polarization transfer curves, the nature of which depends on the CSA and QC values together with the dipolar interactions. The fast oscillation becomes more prominent in the absence of QC and their prominence increases with the CSA values. This indicates that the OPTIANS recouple higher order CSA and dipolar coupling cross-terms to improve the polarization transfer efficiency. This is an important feature that paves the way for the next generation recoupling sequences for materials with large anisotropic nuclear spins. The non-monotonic increment of the OPTIANS efficiency with the strength of the anisotropic interactions, indicates a complex dependence on CSA and QC such that there is a sweet spot in the target range. This could be due to recoupling of multiple higher order terms in the Hamiltonian with different regime of their dominance, however, a more concrete analysis requires rigorous analytical treatment of the pulse.