A quantitative study of the synthesis of metal-organic framework (MOF) colloids via a solvothermal growth process was demonstrated using electrospray-differential mobility analysis (ES-DMA), a gas-phase electrophoresis approach. HKUST-1, a copper-based MOF (Cu-MOF), was selected as the representative MOF of the study. The effects of the synthetic parameters, including ligand concentration (CBTC), synthetic temperature (Ts), and synthetic time (ts) versus material properties of the Cu-MOF, were successfully characterized based on the mobility size distributions measured by ES-DMA. The results show that the mobility size of Cu-MOF was proportional to Ts, ts, and CBTC during the solvothermal growth. X-ray diffraction and Brunauer-Emmett-Teller analyses were employed complementarily to the ES-DMA, confirming that the increase in mobility size of Cu-MOF was correlated to the increase in crystallinity (i.e., larger specific surface area and crystallite size). The results of CO2 pulse adsorption show that the synthesized Cu-MOF possessed a good CO2 adsorption ability under 1 atm, 35 °C, and the cumulative amount of CO2 uptake was proportional to the measured mobility size of Cu-MOF. The work provides a proof of concept for the controlled synthesis of MOF colloids with the support of gas-phase electrophoretic analysis, and the quantitative methodology is useful for the development of MOF-based applications in CO2 capture and utilization.