Gas-source molecular beam epitaxy (GSMBE), designating the method where the group III beams are derived from the evaporation of solid materials while the group V beams are derived from the high-temperature cracking of AsH3 and PH3, is a very promising method. We show in this work that using indium of high purity and optimizing the growth conditions, unintentional impurities in these films prepared by GSMBE can be reduced to a level comparable to that obtained by all-vapor-source chemical beam epitaxy (CBE). The films grown by GSMBE are of very high quality, as deduced from the measurements of electrical, optical, and structural properties. Furthermore, we have found that the alloy composition in InGaAsP for the wavelength λ of 1.1 μm changes significantly in a range of growth temperature from 525 to 530°C, likely due to an abrupt change in the sticking probability of phosphorus. We have also found that the phosphorus-to-gallium flux ratio strongly affects surface morphology of InGaAsP for λ = 1.3 μm.