Low-temperature crystallization to (100)-oriented polycrystalline silicon (poly-Si) thin films is a key requirement for high-performance low-temperature poly-Si thin-film transistors (LTPS-TFTs). Biaxially (100)-oriented poly-Si thin films were formed by multiline beam continuous-wave laser lateral crystallization in single scans. By overlapping scanning, the (100) preferential orientation was stable and (100) silicon crystals were developed over a large area. The crystallinities of the poly-Si films were precisely characterized, especially by two-dimensional X-ray diffraction. It was found that the poly-Si thin films predominantly had (100)-surface-oriented crystals. The crystallinity of the laser-crystallized poly-Si films was dependent on the scanning speed and overlapping condition. The (100) poly-Si films were formed at scanning speeds below the threshold for lateral-crystallized silicon.