In this study, regenerated cellulose fibers were successfully prepared from cellulose/NaOH/thiourea/urea aqueous solution through an efficient extrusion dissolution method. The microstructure of the regenerated cellulose fibers were analysed by using attenuated total reflection infrared (ATR-IR) spectroscopy and the corresponding two-dimensional (2D) correlation spectroscopy. The results showed that the fibers demonstrate a typical crystalline cellulose II and a relatively high crystallinity. Improved crystal structure and tensile strength were obtained in the regenerated cellulose fibers due to improved multi-roller drawing process. The total crystalline index (TCI) and tensile strength of the fibers at different spinning stages were determined in the range of 0.46-0.54 and 1.06-2.30 cN/dtex, respectively. The described cellulose regeneration pathway provided an environmentally friendly and simple method, which could have a significant influence on current cellulose regeneration industries.