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Two-dimensional materials provide opportunities for developing semiconductor applications at atomistic thickness to break the limits of silicon technology. Black phosphorus (BP), as a layered semiconductor with controllable bandgap and high carrier mobility, is one of the most promising candidates for transistor devices at atomistic thickness1–4. However, the lack of large-scale growth greatly hinders its development in devices. Here, we report the growth of ultrathin BP on the centimetre scale through pulsed laser deposition. The unique plasma-activated region induced by laser ablation provides highly desirable conditions for BP cluster formation and transportation5,6, facilitating growth. Furthermore, we fabricated large-scale field-effect transistor arrays on BP films, yielding appealing hole mobility of up to 213 and 617 cm2 V−1 s−1 at 295 and 250 K, respectively. Our results pave the way for further developing BP-based wafer-scale devices with potential applications in the information industry. Centimetre-scale growth of few-layer black phosphorous with high crystalline quality and homogeneity is realized by pulsed laser deposition.