Both phototriggered growth and removal of polymer chains from surfaces are efficient ways to finely tune interface properties. Combining these two capabilities in one system with independent control can significantly increase the feasibility of photoregulation on surface modification but has not been reported yet. Herein we describe a novel approach to control both the growth and the detachment of polymer brushes independently by light with different wavelengths. The approach is based on a nitrodopamine-based initiator (NO2-BDAM) which contains a catechol structure for surface modification, alkyl bromide group for radical polymerization, and o-nitrophenyl ethyl moiety for photolysis. When dimanganese decacarbonyl (Mn2(CO)10) was applied together with NO2-BDAM as an initiating system, visible light (460 nm) can be used to trigger the site-specific growth of polymer brushes. Resulting polymer brushes can be selectively removed by UV light (360 nm). This method is suitable for different monomers on various substrates, suggesting a facile and robust method to regulate surface properties.