Around a quarter of annual worldwide silver consumption comes from recycling. It remains a primary target for researchers to increase the silver ion adsorption capacity of the chelate resin. Herein, a series of flower-like thiourea–formaldehyde microspheres (FTFM) possessing diameters of 15–20 μm were prepared via a one-step reaction under acidic conditions, and the effects of the monomer molar ratio and reaction time on the micro-flower morphology, specific surface area, and silver ion adsorption performance were explored. The nanoflower-like microstructure showed the maximum specific surface area 18.98 ± 0.949 m2/g, which was 55.8 times higher than that of the solid microsphere control. As a result, the maximum silver ion adsorption capacity was 7.95 ± 0.396 mmol/g, which was 10.9 times higher than that of the control. Kinetic studies showed that the equilibrium adsorption amount of FT1F4M was 12.61 ± 0.016 mmol/g, which was 11.6 times higher than that of the control. Additionally, the isotherm study of the adsorption process was performed, and the maximum adsorption capacity of FT1F4M was 18.17 ± 1.28 mmol/g, which was 13.8 times that of the control according to the Langmuir adsorption model. Its high absorption efficiency, convenient preparation strategy, and low cost recommend FTFM bright for further use in industrial applications.