Force-spinning is a popular way to fabricate various fine fibers such as polymer and metal nanofibers, which are being widely employed in medical and industrial manufacture. The spinneret is the key of the device for spinning fibers, and the physical performance and morphology of the spun nanofibers are largely determined by its structure parameters. In this article, the effect of spinneret parameters on the outlet velocity is explored and the spinneret parameters are also optimized to obtain the maximum outlet velocity. The mathematical model of the solution flow in four areas is established at first, and the relationship between outlet velocity and structure parameters is acquired. This model can directly reflect the flow velocity of the solution in each area. Then, the optimal parameters of outlet diameter, bending angle, and curvature radius are obtained combined with the gray wolf algorithm (GWA). It is found that a curved-tube nozzle with a bending angle of 9.1°, nozzle diameter of 0.6 mm, and curvature radius of 10 mm can obtain the maximum outlet velocity and better velocity distribution. Subsequently, the simulation is utilized to analyze and compare the velocity situation of different parameters. Finally, the fiber of 5 wt% PEO solution is manufactured by a straight-tube nozzle and optimized bent-tube nozzle in the laboratory, and the morphology and diameter distribution were observed using a scanning electron microscope (SEM). The results showed that the outlet velocity was dramatically improved after the bent-tube parameters were optimized by GWA, and nanofibers of better surface quality could be obtained using optimized bent-tube nozzles.