This dataset contains experimental data presented in the paper titled 'Passive Pico-injection Enables Controlled Crystallization in a Droplet Microfluidic Device' "Setup.jpg" is the picture of the whole set-up for running the microfluidic device. "Injection-demo.mp4" is the video when blue dye is injected into the moving droplets with DI water. "secondary droplets.mp4" is the video demonstrating the generation of secondary droplets when the flow rate of the side channel is too high. "CaCO3 crystallization.mp4" is the video of CaCO3 crystallization in moving droplets when 100mM Na2CO3 is injected into 100mMCaCl2 droplets with a 1:1 volume ratio. "Calibration of injection volume.xlsx" contains the data of injection volume vs the flow rate of the side channel. "Raman spectra.xlsx" contains the Raman data of (1) standard Raman spectra of amorphous calcium carbonate (ACC), vaterite and calcite prepared in our experiments; (2) ACC formed in the droplets which is suspended in FC-40; and (3) crystals formed at the "Y-junction" when 5mM CaCl2 and 5mM Na2CO3 are combined.