Thin films of La 2 SrCu 2 O 6ϩy with varying Sr/La ratios have been grown by molecular beam epitaxy on ͑001͒ SrTiO 3 ; their structural as well as their transport properties are reported. Under appropriate conditions, thin films with a metal-like resistivity down to 8 K are obtained; i.e., these films are closer to the onset of superconductivity than previous results indicate for bulk samples. This observation might be explained by a thin-film-specific alteration in site occupation of the La and Sr atoms in the lattice. In addition, the defect structures of a typical sample have been studied by transmission electron microscopy and the thin-film/ substrate interface structure is determined. Out-of-phase boundaries with displacement vectors Rϭ͓00 1 5 ͔ occur throughout the entire film thickness. Such interfaces, which possibly originate at substrate surface steps, disconnect the CuO 2 layers and negatively influence eventual superconductivity. The films contain copper oxide outgrowths and nano-sized a-axis grains at the surface. Locally a 2ͱ2a p ϫ2ͱ2a p modulation is observed; we have determined its unit cell and compared it with other so-called 2ͱ2a p ϫ2ͱ2a p structures occurring in other superconducting compounds such as YBa 2 Cu 3 O 7Ϫd and Bi 1.