Light-controlled polymerization has wide applications in additive manufacturing and medicine, but the common catalysts work under UV-blue light, which does not penetrate beyond the surface of the materials or tissues, and may have negative physiological effects. In this work, we demonstrated that perovskite nanocrystals are excellent nonlinear photocatalyst that can be activated with near-infrared light. The giant two-photon absorption coefficient of the nanocrystal, compared with dye molecule catalysts, allows efficient volumetric reaction. Applying a special type of polymerization, PET-RAFT, we showed that the entire solution volume of 1 mL contains polymer chains with highly uniform molecular length (dispersity of 1.07 is very close to unity), which is challenging for conventional laser direct writing. This collaborative work with Egap group at Rice MSNE is published in ACS Macro Letters.