We investigated laser trapping crystallization of glycine by using femtosecond (fs) laser as a trapping light source. Impulsively exerted fs laser pulses crystallized glycine more effectively than that induced by continuous wave (CW) laser trapping. Highly efficient crystallization and crystal growth behavior indicates fs laser irradiation increased the concentration not only at the focal spot, but also around the laser focus. Furthermore, we found that irradiation of fs pulses to CW laser-induced locally high supersaturation region enables immediate crystallization. Spatiotemporally controlled triggering of a single crystal formation with sub-second time resolution has achieved by integrating fs and CW laser trapping techniques.