The preparation of electrospun non‐woven fabrics composed of cellulose and synthetic phosphorylated polypeptides, copoly[Ser(PO3H2)XAspY]s (X:Y = 100:0, 75:25, 50:50, 25:75), is described. The non‐wovens were subjected to an alternate immersion in CaCl2 and Na2HPO4 solutions to induce crystallization of calcium phosphate. The deposited calcium phosphate crystals were analyzed by means of EDX analysis and WXRD. The amounts of calcium phosphate deposition are greater for the cellulose non‐woven fabrics containing copoly[Ser(PO3H2)XAspY] than those of cellulose‐only non‐woven fabrics. These results indicate that copoly[Ser(PO3H2)XAspY] can entrap Ca2+ ions around the fine fiber matrix to accelerate crystallization of the calcium phosphate.magnified image