We have fabricated by pulse laser deposition very thin (∼5-7 nm) and thick (∼27-408 nm) films of composition Fe66B24Nb4Ni6 on silicon and quartz substrates respectively, and studied their magnetic and magneto-optic properties at room temperature. We find that the thicker films on silicon can be tuned by appropriate thermal annealing to exploit soft magnetic characteristics with low HC, and high MS values. The magnetic hysteretic loops of the as-deposited thicker films on silicon substrates show two interesting characteristics: 1) increase in the coercivity with the film thickness and 2) the onset of a two stage process during the approach to magnetic saturation. The initial in-plane characteristic of the hysteresis loop is followed by a linear anisotropic behavior between remanence and saturation- that changes into square soft-magnetic loops on decreasing the film thickness. By suitable annealing the intrinsic strain disappears at relatively low temperatures (≤200°C); the thicker films can be tailored to exhibit a simple soft-magnetic square loop with low HC. The ∼5-7 nm films deposited on glass are transparent and have been investigated for their magneto-optic properties using Faraday rotation (FR) measurement technique. Very high values of FR in the range 4-20 deg/μm almost linearly dependent on the wavelength of light in the range 405-611 nm are observed. The observed high values of Faraday rotation over a wide range of wavelength of light are useful for the applications as magneto-optic sensors in the UV to visible range.