Six pentamethylidene IR dyes with a peak absorption wavelength at 1.06 μm (including two asymmetric dyes) were synthesized for a mode-locking laser. The structure was demonstrated by IR, H1NMR and element analysis. The absorption wavelength varied from 1052 nm to 1095 nm was tested in the solution of 1,2-dichloroethane. A stable laser pulse with a duration of 27～36 ps was observed by using the dyes. The dyes are successfully proved to be used as a collide-pulse mode-locking (CPM) dye for Nd3+:YAG lasers.