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A tapered fiber decorated by Ag nanoparticles is prepared as a surface-enhanced Raman scattering (SERS) substrate. There are two key parameters during the preparation process, the fiber cone angle and the density of decorated AgNPs on the fiber tip surface. Their theoretical analysis on the forming mechanism and the optimization process is studied in detail. The tapered fibers with angles from 0.5 to 30° are successfully prepared, with a chemical method in a small tube using a bending interface. AgNPs with different densities are decorated on the surface of the tapered fibers with an electrostatic adsorption method. The optimized tapered fiber SERS probe with an angle of 12° and AgNPs density of 26.67% provides the detection of Rhodamine 6G (R6G) with 10−10 mol/L.