Abstract: Methods are provided according to aspects of the present invention for making starch fiber or particle compositions by wet-electrospinning or wet-electrospraying including providing a solution or dispersion of starch in an aqueous or non-aqueous solvent or dispersant, where the starch is present at a concentration above the critical entanglement concentration, with the proviso that the aqueous or non-aqueous solvent or dispersant does not consist only of water; heating the solution or dispersion of starch to a temperature above the crystallization temperature of the starch; electro spinning or electro spraying the heated solution or dispersion of starch to produce starch fibers or starch particles, respectively; and contacting the starch fibers or starch particles with a coagulation bath fluid.