Mesoporous aluminas with a uniform fibrous morphology were synthesized using a copolymer-controlled homogeneous precipitation method under hydrothermal conditions. Scanning electron microscopy, X-ray diffraction, solid-state magic-angle spinning nuclear magnetic resonance, transmission electron microscopy, thermogravimetric analysis, nitrogen adsorption, Fourier transform infrared spectrometry, and elemental analysis techniques were used to characterize the samples. The effect of various synthesis conditions on the morphology and mesoporous structure of the alumina fibers was investigated. Such porous alumina microfibers may find applications in nanotechnology and catalysis. They can also be used as advanced high-temperature composite materials and templates for fabrication of fibrous materials of various compositions, such as carbon, transition-metal oxides, and polymers.