This paper reports on the synthesis of birefringent vaterite microspheres with narrow size distribution using a seeded growth method. In a post-treatment the microspheres were stabilized and functionalized through coating with a combination of organosilica and silica. The coating vastly enhanced the stability of the vaterite microspheres in biological buffers and allowed the attachment of biomolecules such as DNA or proteins. As an example, streptavidin was attached to the surface of the functionalized microspheres. These results pave the way for the use of birefringent vaterite particles for the micromanipulation of single biological molecules such as DNA or specific proteins in an optical trap capable of exerting and measuring torques. The stabilized birefringent microspheres may also find use for biosensor and biological screening applications.