Summary: Homopolymers and a series of copolymers with tris‐8‐hydroxyquinoline aluminum (Alq3) as the cross‐links are synthesized. All these polymers show improved electroluminescence (EL) efficiency over their previously reported counterparts. Among them, the copolymers containing Alq3 and carbazole groups show higher EL efficiency than that of the homopolymers. We also demonstrate the feasibility of generating patterns using the homopolymers via photopolymerization. The cross‐linked nature, selectivity of patterning, high thermal stability, and EL efficiency might render these polymers a promising material in fabricating large‐scaled multilayered sub‐pixellation organic light‐emitting diodes (OLEDs).