This study reports the synthesis of tail-shaped alginate particles using a microfluidic platform combined with a sedimentation strategy. By utilizing microfluidic emulsification in the cross-junction channel, the formation of regular droplets was achieved. Following a facile and convenient sedimentation process and an ionic crosslinking process, sodium-alginate droplets became tail-shaped and then gradually developed into calcium-alginate microparticles. The effects of the concentration of the CaCl2 crosslinker and the viscosity of the alginate solution on the shape and/or size of the particles were further investigated. The proposed synthesis methodology has the advantages of actively controlling the tail-shape formation, having a narrow size distribution, as well as being a facile and convenient process with a high throughput. This approach can be applied to many applications in the pharmaceutical and biomedical arena.