Niobium diselenide has potential for use as a solid lubricant, but to achieve the optimal properties of low friction coefficient, high conductivity and oxidation resistance, the Se/Nb ratio and crystallinity must be carefully controlled. It has been shown that pulsed laser deposition (PLD) permits the required degree of control, even over films with complex stoichiometries. In this study, a designed experimental approach was chosen to look at the major trends across the upper and lower limits of the PLD process for niobium diselenide. Film chemistry and crystallinity were evaluated using X-ray photoelectron spectroscopy, Rutherford backscattering spectroscopy, and glancing-angle X-ray diffraction. This study has shown that film chemistry can be changed from substoichiometric to superstoichiometric, and crystallinity varied between amorphous and crystalline, by appropriate choice of PLD parameters. The property correlations developed and the acquisition system used will be described.