There is provided a method capable of manufacturing a mold at low cost, and a method of manufacturing a biocompatible pattern sheet by using the mold. The method of manufacturing a mold 68 having a recessed pattern 70 includes the steps of: forming a silicone resin film 60 by applying a silicone resin solution 58 to a surface of a model 40 having a protrusion pattern 42; defoaming the silicone resin film 60 by reducing the silicone resin film 60 in pressure; forming the mold 68 by heating and curing the silicone resin film 60 while a base plate 64 is in contact with a face of the silicone resin film 60, the face being opposite to the model 40; and releasing the mold 68 from the model 40 after releasing the base plate 64. The method of manufacturing a pattern sheet 76 uses the mold 68.