Two-photon-pumped dye lasers are very important because of their applications in wavelength up-conversion, optical data storage, biological imaging and photodynamic therapy. Such lasers are very difficult to realize in the solid state because of the aggregation-caused quenching. Here we demonstrate a new two-photon-pumped micro-laser by encapsulating the cationic pyridinium hemicyanine dye into an anionic metal-organic framework (MOF). The resultant MOF [symbol: see text] dye composite exhibits significant two-photon fluorescence because of the large absorption cross-section and the encapsulation-enhanced luminescent efficiency of the dye. Furthermore, the well-faceted MOF crystal serves as a natural Fabry-Perot resonance cavity, leading to lasing around 640 nm when pumped with a 1064-nm pulse laser. This strategy not only combines the crystalline benefit of MOFs and luminescent behaviour of organic dyes but also creates a new synergistic two-photon-pumped lasing functionality, opening a new avenue for the future creation of solid-state photonic materials and devices.