Chiral films stacked with a twist angle can have strong and tunable chiroptical properties and are thus useful for applications such as 3D optical displays, enantioselective catalysis and chiral sensing. However, when it comes to the actual preparation of these chiral films, there are more than 108 potential combinations of the huge number of variables involved — such as the choice of constituent materials, film thickness and strain, and twist angle. Trial and error is simply not efficient enough to find optimal chiroptical activities within this expansive design space. Gang Zou, Xin Chen, Jun Jiang and colleagues use an artificial-intelligence-guided robot to accelerate the discovery and fabrication of target chiral functional films. As one application, the robot is able to design and synthesize a series of tunable, circularly polarized luminescent films made from achiral perovskite quantum dots.