Hypromellose (HPMC)-based hydrophilic composites (HCs) used for rapid dissolution of ferulic acid (FA) were investigated. Electrospun and casting HCs were prepared from a solution containing HPMC, FA, and polyethylene glycol. Ethanol was used as sheath fluid during coaxial processes, and the effects of its flow rates on the Taylor cone and straight fluid jet were investigated. The morphology, component state, hydrophilicity, and drug dissolution rate of the HCs were characterized. Results demonstrated that all HCs were amorphous materials, and their components were compatible. However, the dissolution rate of electrospun HCs was 10 times faster than that of casting HCs. The smaller the diameters of electrospun HCs were, the better their performances were. The mechanism of electrospun HCs was suggested. By utilizing modified coaxial electrospinning and combinations of drug carriers, new types of HPMC-based HCs can provide an alternative approach for the effective delivery of poorly water-soluble drugs.