Fabricating one-dimensional (1D) single-crystalline nanostructures with the necessary characteristics for interconnects and functional units in nanodevices poses a major challenge. Traditional solution-based synthesis methods, driven by oriented attachment mechanisms, have limited the growth of either ultrathin crystalline nanowires or short rod-like nanocrystals due to stringent orientation requirements. The construction of single-crystalline ultralong nanowires with both an elongated length and moderate thickness has remained elusive. Here we introduce a growth mechanism based on progressively oriented attachment that enables the attachment of larger crystals while preserving the alignment of the crystal lattice. Using this mechanism, we achieve 1D single-crystalline lanthanide-doped nanowires (K2YF5:Yb/Er) with lengths up to 9 μm and a moderate thickness of approximately 20 nm. These nanowires can be integrated into a flexible film that exhibits stretching-dependent upconverted luminescence behavior. The mechanical toughness and elongated morphology of the nanowires facilitate the development of a wearable device dedicated to multidirectional strain sensing with high responsivity and excellent stability, withstanding repeated stretching and releasing for up to 1000 cycles.