Using theoretical simulations for optical fiber surface plasmon resonance (SPR) sensors and prism-based SPR sensors coated with negative permittivity material (NPM), we investigated the effect of the permittivity of NPM on the transmitted spectrum of optical fiber SPR sensors and the reflected spectrum of prism-based SPR sensors and then obtained optimum permittivity of the NPM, which can excite the sharpest SPR spectrum in the white light region (400–900 nm).