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In the present work, we have investigated the capability of different bimetallic combinations to be used in a fiber optic sensor based on the technique of surface plasmon resonance. The metals considered for the present analysis are silver, gold, copper, and aluminum. The performance of the sensor with different bimetallic combinations is evaluated and compared numerically. The performance is analyzed in terms of three parameters: sensitivity, signal-to-noise ratio (SNR), and operating range. On the basis of the comparison and some logical criteria, the best possible bimetallic combination along with requisite thickness distribution is predicted. The bimetallic combination is capable of simultaneously providing the larger values of sensitivity, SNR, and operating range, which is not possible with any single metallic layer.