A superhydrophobic surface of modified silica composite was prepared on cotton substrates using a low-temperature process. It is believed that the hydrophobic and self-assembling properties of hexadecyl groups, together with the grainy structure of the surface, convert the cotton surface from superhydrophilic to superhydrophobic. The maintenance of the hydrophobic properties of the coating after repeated washing is attributed to the linking ability of GPTMS that promote a high level of adhesion at the interface. Investigations of the mechanical and physical properties of cotton before and after coating show no adverse effect of the coating to cotton substrates with respect to strength and permeability. This surface-finishing process could be used to produce environmentally friendly superhydrophobic surfaces for a wide variety of materials.