Material composition engineering and device fabrication of perovskite nanocrystals (PNCs) in solution can introduce organic contamination and entail several synthetic, processing, and stabilization steps. We report three-dimensional (3D) direct lithography of PNCs with tunable composition and bandgap in glass. The halide ion distribution was controlled at the nanoscale with ultrafast laser–induced liquid nanophase separation. The PNCs exhibit notable stability against ultraviolet irradiation, organic solution, and high temperatures (up to 250°C). Printed 3D structures in glass were used for optical storage, micro–light emitting diodes, and holographic displays. The proposed mechanisms of both PNC formation and composition tunability were verified.