Quantum computing is the field of science that uses quantum-mechanical phenomena, such as superposition and entanglement, to perform operations on data. The fundamental information unit used in quantum computing is the quantum bit or qubit. It is well-known that quantum computers could theoretically be able to solve problems much more quickly than any classical computers. Currently, the first and still the most successful implementations of quantum information processing (QIP) have been based on nuclear spins in liquids. However, molecules that enable many qubits NMR QIP implementations should meet some conditions: have large chemical shifts and be appropriately dispersed for qubit addressability, appreciable spinspin coupling between any pair of spins, and a long relaxation time. In this line, benzyldene-2,3-dihydro-1H-[1,3]diphosphole (BDF) derivatives have been theoretically tested for maximizing large chemical shifts, spinspin coupling, and minimizing the hyperfine coupling constant. Thus, the structures were optimized at the B3LYP/6-311G(d,p) level and showed a significant similarity with the experimental geometrical parameters. The NMR spectroscopic parameters (delta and J) were calculated with six different DFT functionals. The tau-HCTH/6-31G(2d) level is in better agreement with the experimental data of P-31 and C-13 chemical shifts, while PCM-B3LYP/cc-pVDZ level shows a decrease on deviation between calculated and experimental values for PP and PC SSCC. The surface response technique was employed to rationalize how the hyperfine constant varies with the chemical shifts and coupling constants values. From our findings, BDF-NO2 was the best candidate for NMR quantum computations (NMR-QC) among the studied series.