A method for manufacturing a honeycomb structure includes a molding step of manufacturing a pillar-shaped honeycomb molded body by using a raw material composition, and a firing step of carrying out a firing treatment on the honeycomb molded body to manufacture a honeycomb fired body. The pillar-shaped honeycomb molded body has a large number of cells disposed in substantially parallel with one another in a longitudinal direction with a cell wall therebetween. The raw material composition includes inorganic particles, at least one of inorganic fibers and inorganic whiskers, and an inorganic binder. The inorganic particles include secondary particles formed by an agglomeration of primary particles. An average particle diameter of the inorganic binder in the raw material composition is about 1/200 to about 1/40 of an average particle diameter of the inorganic particles.