Poly(siloxane-ether-urethane)-acrylic (PU-AC) hybrid emulsions were prepared by introducing different hydroxyethoxypropyl-terminated polydimethylsiloxane (PDMS) content into the acrylic-terminated poly(ether-urethane) backbone and then in situ copolymerizing with methyl methacrylate and butyl acrylate via emulsion process. The effects of PDMS on the particle size and viscoelastic behavior of the hybrid emulsions were investigated. Meanwhile, the hydrogen bonding, mechanical and thermal mechanical properties, water resistance, the surface gloss, and wettability of the resultant hybrid films were also studied. The results showed that all the hybrid emulsions showed shear-thinning behaviors, and the introduction of PDMS resulted in the formation of the hybrid emulsions with increased average particle size and decreased viscosity. The chemical bonds built between PU and AC yielded higher than 73% crosslinking fraction in all the hybrid materials, but this value decreased with increasing PDMS content because PDMS reduced the hydrogen bonding interactions and enhanced the phase separation. As a result, an increase in the PDMS content led to an increase in the elongation, water resistance, surface roughness, and water hydrophobic of the films, but the tensile strength, hardness, storage modulus, and glass transitions temperature decreased. It is suggested that introduction of PDMS can provide the hybrid materials with the improved flexibility, water resistance, and surface hydrophobicity, which has potential application value in the fouling-release coatings, biomaterials, and surface fishing.