Liquid crystal elastomers (LCEs) are polymer networks that exhibit anisotropic liquid crystalline properties while maintaining the properties of elastomers, presenting reversible high-speed and large-scale actuation in response to external stimuli. Herein, we formulated a non-toxic, low-temperature liquid crystal (LC) ink for temperature-controlled direct ink writing 3D printing. The rheological properties of the LC ink were verified under different temperatures given the phase transition temperature of 63 °C measured by the DSC test. Afterwards, the effects of printing speed, printing temperature, and actuation temperature on the actuation strain of printed LCEs structures were investigated within adjustable ranges. In addition, it was demonstrated that the printing direction can modulate the LCEs to exhibit different actuation behaviors. Finally, by sequentially conforming structures and programming the printing parameters, it showed the deformation behavior of a variety of complex structures. By integrating with 4D printing and digital device architectures, this unique reversible deformation property will help LCEs presented here apply to mechanical actuators, smart surfaces, micro-robots, etc.