Enzyme Immobilization In article number 2406097, Fernando López-Gallego and co-workers develop a universal method for encapsulating single gram-negative microbes with polymeric coatings to fabricate synthetic spores that selectively bind His-tagged enzymes. These synthetic spores serve as biocatalytic materials for the one-pot oxidative amination of diols into amino alcohols, facilitated by the cooperative catalysis between intracellular and extracellular enzymes that maintain their performance in consecutive batch cycles.