A method of coating surfaces of various body-implantable materials with control-releasable nitrogen monoxide using a catecholamine, more particularly, technology of preparing a coating film containing a diazeniumdiolate functional group on a surface of a material to be coated using a catecholamine, is provided. The coating film prepared by the method has advantages in that nitrogen monoxide can be stably supplied under an in vivo environment, and can be suitably used in a living body without causing cytotoxicity. Therefore, among the materials having a coating film formed on a surface thereof, the body-implantable material is especially expected to be widely used for medical and health applications including treatment of ischemic disorders such as arteriosclerosis through controlled release of nitrogen monoxide, regulation of penile erections, antibacterial and antiviral effects, and wound healing.