In this work, we adopted pulsed laser deposition (PLD) with a Nd:YAG laser to develop Bi1−xGdxFeO3 (BGFO) films on glass substrates. The phase composition, microstructure, ferroelectric, magnetic, and nanomechanical properties of BGFO films are studied. BGFO films with x = 0.00–0.15 were confirmed to mainly consist of the perovskite phase. The structure is transformed from rhombohedral for x = 0.00 to pseudo-cubic for x = 0.05–0.10, and an additional phase, orthorhombic, is coexisted for x = 0.15. With increasing Gd content, the microstructure and surface morphology analysis shows a gradual decrease in crystallite size and surface roughness. The hardness of 5.9–8.3 GPa, measured by nanoindentor, is mainly dominated by crystallized structure and grain size. Good ferroelectric properties are found for BGFO films with x =0.00–0.15, where the largest remanent polarization (2Pr) of 133.5 µC/cm2 is achieved for x = 0.10, related to low leakage and high BGFO(110) texture. The improved magnetic properties with the significant enhancement of saturation magnetization from 4.9 emu/cm3 for x = 0 to 23.9 emu/cm3 for x = 0.15 by Gd substitution is found and related to large magnetic moment of Gd3+ and suppressed spiral spin structure of G-type antiferromagnetism. Furthermore, we also discuss the mechanisms of leakage behavior as well as nanomechanical characterizations as a function of the Gd content.