In this paper, a systematic technique is proposed for the optimal placement and design of nonlinear dampers for building structures. The concept of Output Frequency Response Function (OFRF) is applied to analytically represent the output frequency response of a building frame where nonlinear viscous dampers are fitted for suppression of vibration during earthquakes. An effective algorithm is derived using the analytical representation to optimally determine the locations and parameters of the nonlinear dampers. Various numerical examples are provided to verify the effectiveness of the optimal designs. A comparison of the vibration suppression performance with that of the frame structure under a random or uniform damping allocation is also made to demonstrate the advantages of the new designs over traditional solutions.