Solution-processed multilayered OLEDs are fabricated through a conceptually novel, simple, intelligent, and cost-effective strategy, namely "layer-by-layer cross-linking" (LBLX). It enables the use of a wide range of conventional and low-priced wet deposition techniques (e.g., all printing techniques), and is based on "PEDOT-initiated cross-linking" of oxetane-functionalized polymers, which resembles the "grafting-from" approach.