Liquid crystalline elastomer (LCE)-based microparticles that can change shapes in response to external stimuli are of great interest for potential applications such as artificial cells, micro-actuators, micro-valves, and smart drug carriers. Here, the synthesis of LCE microparticles with diverse temperature-dependent anisotropic shapes originated from the same Janus microdroplets is reported. The Janus microdroplets, suspended in an aqueous solution of surfactants, are transformed from microdroplets consisting of a mixture of liquid crystal (LC) monomers, oligomers, silicone oil, and an organic solvent, after the removal of the organic solvent. The molecular alignment of the LC part at the interface, whether planar, homeotropic, or hybrid, is dependent on the choice of the surfactants but not affected by the silicone oil. After polymerization and solvent extraction of the unreacted components, LCE microparticles of various shapes are obtained depending on the concentration and composition of the surfactants, the weight ratio of the LC part to the silicone oil part, and the choice of the extraction solvent. The microparticles that undergo different synthetic pathways show distinct thermally responsive shapes, much like how stem cells differentiate in different environmental conditions.