The homo- and heteroepitaxial deposition of LGS (langasite, La3Ga5SiO14) thin films on LGS single crystals, Si and SiO2 substrates by pulsed laser deposition (PLD) is demonstrated. PLD is performed at substrate temperatures up to about 700 °C and results initially in Ga deficient films. Two strategies of counterbalancing the Ga deficit are realized. First, off-stoichiometric targets with an enhanced Ga content are applied. Secondly, an increased oxygen partial pressure up to about 6 Pa is used during deposition to suppress evaporation of Ga suboxides. Combining these adaptions results in the growth of stoichiometric LGS thin films. Films deposited on LGS substrates do not show any additional X-ray diffraction reflexes nor broadening of the peaks with respect to the single crystalline substrates. Therefore, the homoepitaxial approach can be considered successful. The deposition on Si and SiO2 substrates under the same conditions leads to the formation of polycrystalline films. However, post-annealing at 800 °C increases crystallinity. Stoichiometry and homogeneous distribution of La, Ga and Si cations are confirmed by secondary neutral mass spectrometry (SNMS). The composition remains constant within the film, implying stable process parameters.