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An enzymatic tandem reaction is described in which the enzymes phosphorylase and Deinococcus geothermalis glycogen branching enzyme (Dg GBE) catalyze the synthesis of branched polyglucans from glucose-1-phosphate (G-1-P). Phosphorylase consumes G-1-P and polymerizes linear amylose while Dg GBE introduces branching points on the α-(1→6) positions by reshuffling short oligosaccharides. The resulting branched polyglucans have an unusually high degree of branching of 11%.