The main commercially used birefringent oxides a-BaB 2 O 4 and YVO 4 have the birefringences of 0.12 and 0.22. We propose atargeted high-throughput screening system to search birefringence-active functional modules (FMs) and large birefringent materials.Aseries of p-conjugated CÀOu nits 2À are discoveredt o be birefringence-active FMs.T heoretical and experimental studies on the crystals with C À Ounits confirm the feasibility of strategy.B ased on this,t he CÀOc ontaining compounds ranging from deep-ultraviolet to near-infrared region with large birefringence from 0.1 to 1.35 are found, and most of them break through the birefringent limit of oxides.T he (NH 4 ) 2 C 2 O 4 •H 2 Oc rystal is grown and its experimental birefringence is 0.248 at 546 nm, which is identified as apromising UV birefringent crystal. The A-site cations playsignificant roles in optical properties by influencing the density and arrangement of the CÀOunits.