Organolead trihalide perovskites have emerged as a new class of competitive solution-processed semiconductors due to their unique optoelectronic properties. However, poor ambient stability and charge transport are the Achilles’ heel of hybrid perovskites, thus limiting their applications. In this work, microwave-assisted synthesis is applied for the first time to rapidly grow perovskite single crystals embedded with single-wall carbon nanotubes. These nanotube-in-perovskite single crystals are endowed with a carrier mobility one order of magnitude higher than the pure counterpart and the related photodetectors show an ultrafast photo-response speed (5 and 80 ns for rise and decay time, respectively). The fast and uniform heating of microwave irradiation facilitates the synthesis of ambient-stable crystals with nanoscale additives, paving the way to creating a wide range of mixed-dimensional perovskite-based nanocomposites with optimal properties and device performance.