Organic−inorganic metal halide perovskites have recently attracted increasing attention as highly efficient light harvesting materials for photovoltaic applications. The solution processability of these materials is one of their major advantages on the route toward fabrication of low-cost solar cells and optoelectronic devices. However, the precise control of crystallization and morphology of organometallic perovskites deposited from solutions, considered crucial for enhancing the final photovoltaic performance, still remains challenging. In this context, here, we report on growing microcrystalline deposits of methylammonium lead triiodide perovskite, CH3NH3PbI3 (MAPbI3), by one-step solution casting on cylinder-shaped quartz substrates (rods) having diameters in the range of 80 to 1800 μm. We show that the substrate curvature has a strong influence on morphology of the obtained polycrystalline deposits of MAPbI3. Specifically, a marked size reduction of MAPbI3 microcrystallites concomitant with an increased crystal packing density was observed with increasing the substrate curvatures. In contrast, although the crystallite width and length markedly decreased for substrates with higher curvatures, the photoluminescence (PL) spectral peak positions did not significantly evolve for MAPbI3 deposits on substrates with different diameters. The crystallite size reduction and a denser coverage of microcrystalline MAPbI3 deposits on cylinder-shaped substrates with higher curvatures were attributed to two major contributions, both related to the annealing step of the MAPbI3 deposits. In particular, the diameter-dependent variability of the heat capacities and the substrate curvature-enhanced solvent evaporation rate seemed to contribute the most to the crystallization process and the resulting morphology changes of MAPbI3 deposits on cylinder-shaped quartz substrates with various diameters. The longitudinal geometry of cylinder-shaped substrates provided also a facile solution for checking the PL response of the deposits of MAPbI3 exposed to the flow of various gaseous media, such as oxygen (O2), nitrogen (N2), and argon (Ar). Specifically, under excitation with λexc = 546 nm, the rapid and pronounced decreases and increases of PL signals were observed under intermittent subsequent exposures to O2 and N2, respectively. Overall, the approach reported herein inspires novel, cylinder-shaped geometries of MAPbI3 deposits, which can find applications in low-cost photo-optical devices, including gas sensors.