Drop-based microcavity lasers emerged as a promising tool in modern physics investigation and chemical detection owing to their cost-effective fabrication, high luminescence, and sensitive molecule sensing. However, it is of great challenge to achieve highly directional emission along with high quality (Q) factors via traditional droplet self-assembly behavior of the gain medium on a planar substrate. In this work, a single-mode microcavity laser with directional far-field emission is first proposed via droplet self-assembly 3D-curved microcavities, and simultaneously, acetic acid (AcOH) gas sensing is realized. Trichromatic single-mode lasing in 3D-curved microcavities with distinct organic polymer droplets is constructed on silica fibers via a self-assembly procedure. By regulating the curvature of the substrate, mode selection and directional emission of the lasing action are realized. The measured Q-factor of the proposed anisotropic 3D-curved active microcavity is ∼20k. Furthermore, on account of the sensitive responsiveness of liquid organic polymers, single-mode laser sensors can be realized by measuring the shift of their lasing modes on exposure to organic vapor. Benefiting from chemical reaction with rhodamine 6G, the AcOH gas sensor displays a short response time. These results may open new insights into drop-based quasi-3D-anisotropic whispering-gallery-mode microcavities to improve the development of lab-in-a-droplet, ranging from a tuneable microcavity laser to a chemical gas sensor.