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We report a robust route to the one‐pot synthesis of Ag icosahedral nanocrystals with uniform and controllable sizes. Our results indicate that multiply‐twinned seeds are initially formedviahomogeneous nucleation, followed by their growth into icosahedral nanocrystals with enlarged sizes. During the growth process, Ostwald ripening plays a key role in enabling the formation of nanocrystals with a narrow size distribution. In addition to the conventional approach involving the variation of reaction time, we are able to control the size of the icosahedral nanocrystals by adjusting the molar ratio of the Ag(I) precursor to the reducing agent, altering the reaction temperature, and/or introducing additional Ag(I) precursor. The Ag icosahedral nanocrystals embrace strong localized surface plasmon resonance, with a tunable peak position depending on the particle size. We believe the availability of Ag icosahedral nanocrystals with uniform, tunable sizes offers a great opportunity to investigate their plasmonic and catalytic properties, as well as related applications.