MetglasTM 2826MB foils of 25–30 μm thickness with the composition of Fe40Ni38Mo4B18 have been used for magnetoelastic sensors in various applications over many years. This work is directed at the investigation of ∼3 μm thick iron-nickel-molybdenum-boron (FeNiMoB) thin films that are intended for integrated microsystems. The films are deposited on Si substrate by co-sputtering of iron-nickel (FeNi), molybdenum (Mo), and boron (B) targets. The results show that dopants of Mo and B can significantly change the microstructure and magnetic properties of FeNi materials. When FeNi is doped with only Mo its crystal structure changes from polycrystalline to amorphous with the increase of dopant concentration; the transition point is found at about 10 at. % of Mo content. A significant change in anisotropic magnetic properties of FeNi is also observed as the Mo dopant level increases. The coercivity of FeNi films doped with Mo decreases to a value less than one third of the value without dopant. Doping the FeNi with B together with Mo considerably decreases the value of coercivity and the out-of-plane magnetic anisotropy properties, and it also greatly changes the microstructure of the material. In addition, doping B to FeNiMo remarkably reduces the remanence of the material. The film material that is fabricated using an optimized process is magnetically as soft as amorphous MetglasTM 2826MB with a coercivity of less than 40 Am−1. The findings of this study provide us a better understanding of the effects of the compositions and microstructure of FeNiMoB thin film materials on their magnetic properties.