A method of manufacturing a needle-like array sheet includes supplying a first needle-like array-forming solution consisting of an aqueous solution on a first mold having a first recess; interrupting drying in a wet state and forming a needle-like distal end part; supplying a second needle-like array-forming solution consisting of an aqueous solution on a second mold having a second recess; peeling a sheet part molding product, which is dried and solidified and has a protrusion corresponding to the second recess, after the sheet part molding product is formed; inserting the protrusion of the sheet part molding product into the first recess of the first mold; drying and solidifying the needle-like distal end part and the sheet part molding product after inserting the protrusion, bonding the needle-like distal end part and the protrusion of the sheet part molding product together, and forming a needle-like array sheet having the needle-like array.